Highly reconfigurable neuronlike conductive networks through nanophase structure engineering

Domain: neuroscience
Published: 2025-12-29
Editorial outcome: minor_revision

Abstract
Bionic electronics are designed to bridge the gap between biological systems and conventional electronic devices. However, replicating the high dynamic adaptivity and functional plasticity of living tissues while preserving the electrical performance and structural integrity of tradition electronics remains highly challenging, owing to the intrinsic trade-offs in molecular design. To address this issue, a methodology of reversible nanophase regulation is proposed, inspired by ion-specific effects in biological environments. Benefiting from the dynamic response of noncovalent interaction to specific ions, the developed system can successfully integrate multiple traditionally contradictory properties – combining outstanding electrical/mechanical performance with excellent reconfigurability, such as re-writability of conductive pathways, in-situ wet solderability with good spatial resolution, and closed-loop recyclability. This methodology offers a promising framework for designing reconfigurable devices for bioelectronics applications such as human-machine integration and tissue engineering.

Introduction
Bionic electronics aim to merge biological living organisms and conventional electronic devices, with great promise in applications such as wearable/implantable intelligent devices1, tissue engineering2, human-machine interaction3, and neurorobotics4. However, most conventional electronic devices struggle to replicate the intrinsic reconfigurability and responsiveness of biological living tissues at the hardware level5–7. For example, the brains encode and remove memories by strengthening or weakening synaptic connections between neurons through trans-synaptic proteins such as neurexins (presynaptic) and neuroligins (postsynaptic)8,9 (Fig. 1a). In contrast, traditional electronics are typically incapable of reconfiguring their circuitry once fabricated, resulting in limited functional plasticity across spatial and temporal dimensions.

To offer reconfigurability to electronics, two strategies at different spatial scales were proposed, i.e., macroscopic geometric regulation and molecular structure (or doping level) regulation. Based on these two strategies, several reconfigurable devices were developed, with examples ranging from the adjustable antennae based on mechanical stretching10,11, rewritable conductive hydrogel by controlling their swelling degrees12–15 to active optical metasurface devices based on dynamic conducting polymer16,17 and neuromorphic devices by engineering ion migration and electron transport18–20. Unfortunately, these two strategies struggled to integrate reconfigurability with excellent electrical performance and size scalability, inferior to bulky but delicate living organisms. This issue is mainly rooted in an intrinsic conflict in material design, where the high electrical performance usually requires electrical materials to have highly conjugated or crystalline molecular structures with intimate electrical contacts, while the high reconfigurability usually necessitates weak and responsive intermolecular interaction. For instance, light-responsive conductive hydrogel could be constructed through host-guest interaction, but suffered from a low electrical conductance or structural compactness15. Therefore, bionic reconfigurable electronics sharing a similar physiological mechanism to organisms are highly demanded and challenging.

The specific ion effect, encompassing the popular Hofmeister series, has long been found to strongly affect a range of biological processes such as neuron activity, mainly originating from electrostatic interaction, hydration effects, and/or molecular sieve effects21,22. Inspired by this biological mechanism, we herein propose a general strategy, reversible nanophase regulation of non-covalent crosslinking networks, to successfully construct neuron-mimicking highly-reconfigurable conductive networks (Rec-CN) (Fig. 1a). As an exemplary model, physically crosslinked conductive networks are prepared with conducting polymer, poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS, CP), and polyvinyl alcohol (PVA) as building blocks (Fig. 1b). By leveraging specific ion effect, the conductive network could be finely engineered, either locally or globally, to transition among different thermodynamic states with different nanophase structures, driven by the delicate balance of inter- and intra-molecular non-covalent interactions of polymers (Fig. 1b). The unique capability enabled controlled spatial modulation of electrical conductivity within a single system over a remarkable range of 4–5 orders of magnitude, without compromising structural integrity and mechanical robustness (Fig. 1c–e).

Moreover, owing to the high reconfigurability, in-situ wet soldering and closed-loop recycling could also be realized. In the in-situ wet soldering, the Rec-CN could be directly joined to diverse substrates via laser process or thermal treatment, while preserving its multichannel electrical connections and 3-dimensional (3D) geometric integrity, standing in contrast to previously reported hydrogel soldering methods, which typically required intricate manual operation or were incompatible with 3D gels (Fig. 1f, g)23. In the closed-loop recycling, the Rec-CN could also be recycled in a nearly closed loop through dialysis and heating, with no significant loss in mechanical and electrical properties. Last, benefiting from these unique features, the Rec-CN were therefore demonstrated for the application of various bioelectronics and wearable electronics, including a reconfigurable printing circuit board (Rec-PCB), an on-body wrist for electrophysiological signal capture, and rewritable electroluminescent devices.

As a whole, we propose a reversible nanophase regulation strategy to address a critical methodology gap in bridging the spatial scales for the in-situ regulation of electrical performance in reconfigurable electronics. As a result, this approach successfully integrates good electrical and mechanical performance without standing reconfigurability features, such as micro-pattern ability and re-writability of conductive pathways, in-situ wet solderability with good spatial resolution, and closed-loop recyclability. This strategy also shows great compatibility with other material systems, such as metal-based elastomers and insulative components with ion-specific effects, shedding light on the design of bionic next-generation electronics. Additionally, this work successfully demonstrates that specific ion effects can be utilized to delicately in situ tune the physical properties of noncovalent networks through nanophase structure engineering, providing an efficient toolbox for the mechanism study of polymer-based functional composites, especially for the volatile or degradable system where the employment of the conventional time-temperature superposition principle may be restrained.

Results
Material design, electrical, and mechanical performances
Conductive organogels were constructed as exemplary reconfigurable models by employing CP, PVA, and glycerol as conductive filler, phase-regulating components, and dispersed medium, respectively. In mechanism design, CP and PVA were able to offer abundant hydrogen bonds and electrostatic interactions that were susceptible to specific ion effects, thus benefiting the reconfigurability of polymer networks, whereas glycerol could serve as both a plasticizer to prevent over-dense stacking of CP and PVA for higher dynamics and a lowly volatile medium for expanded working temperature windows. Unless otherwise specified, for the preparation of the organogels, suspensions containing different ratios of CP and PVA, with 4 wt% glycerol, were drop-casted on substrates and then partially dried under ambient conditions (25°C, 50% relative humidity) for 24 h. During this drying process, most water was selectively evaporated, leaving behind pristine CP-PVA organogels (p-CP-PVA) with solid contents of ~40 wt% and residual water contents of 22 wt% (relative to the total mass of organogels) (Supplementary Fig. 1). The influence of environmental humidity during drying is discussed in Supplementary Note 1 and summarized in Supplementary Table 1.

The p-CP-PVA organogels were free-standing and exhibited varied mechanical robustness depending on the relative contents of each component (Supplementary Note 2 and Supplementary Figs. 2–4). For the electrical performance, the p-CP-PVA organogels were almost non-electronically-conductive, as measured by a significantly low conductivity of 0.46–0.73 mS cm−1 (Supplementary Fig. 5). To improve the conductance, mild thermal annealing was implemented in ambient environment, with an optimum annealing temperature of 80°C and duration of 2 h selected based on organogel stability and experimental reproducibility (Supplementary Note 3, Supplementary Fig. 6). The resultant organogels (CP-PVA) experienced significant improvement by 4–5 orders of magnitude, reaching 4.6-112.5 S cm−1 depending on the CP’s contents in the organogels, accompanied by moderate improvement in mechanical performance and increase in solid content of ~50 wt% (Fig. 2a–d and Supplementary Figs. 6 and 7). Notably, the thermal annealing was largely insensitive to environmental humidity, as revealed by the comparable low residual water contents (~4%) in organogels treated under different relative humidity levels (20–70%) (Supplementary Note 1, Supplementary Fig. 8 and Supplementary Table. 1). Moreover, the conductivities of organogels showed low dependency on the gel thickness in a wider range of 0.3–1.0 μm, confirming the uniform distribution of CP within the organogel matrix (Supplementary Note 4 and Supplementary Fig. 9).

More importantly, when compared with the pure PVA organogel, the thermally-annealed CP-PVA organogel exhibited unexpected improvement in mechanical performance, which is in sharp contrast to most previous reports where the incorporation of rigid conductive fillers typically led to embrittlement of the composites (See detailed comparison in Supplementary Table 2). Specifically, with increasing the CP content from 0 to 16 wt% (relative to the total mass of CP and PVA), the CP-PVA organogels exhibited simultaneous increases in Young’s modulus, fracture strain, strength, and toughness by 208.3% (2.4–7.4 MPa), 30.4% (761–992%), 70.6% (6.8–11.6 MPa) and 145.5% (32.5–79.8 MJ m−3), respectively (Fig. 2c, d, Supplementary Fig. 7). As a result, the PVA-CP organogels exhibited superior comprehensive performance in terms of conductivity, stretchability, and toughness when compared with previously reported conducting polymer hydrogels (Fig. 2e, f, Supplementary Fig. 10 and Supplementary Table 3). Furthermore, the CP-PVA organogels exhibited satisfactory conductance retention upon tensile strain, as shown by low increases in resistance by only 0.04, 0.22, and 1.20 times at the strains of 50%, 100%, and 200%, respectively (Supplementary Fig. 11).

At last, the CP-PVA organogels exhibited higher resistance to environmental humidity and high/low temperature than their hydrogel counterpart with only water as the dispersed medium, due to the low volatility of glycerol (Supplementary Figs. 12–20 and Supplementary Note 5). For example, upon exposure to a high-temperature environment of 80°C, the CP-PVA organogels showed satisfactory stability in terms of mechanical and electrical properties. Such high intactness could not only enhance the system’s reliability but also greatly expand the methodological toolbox for rational control over the conductive network by regulating nanophase structure, a key for the reconfigurable system as elaborated below.

Mechanism for the formation of bicontinuous phase
The successful decoupling of electrical and mechanical performances of the CP-PVA organogel could be attributed to the formation of a bicontinuous nanophase structure composed of PVA-rich and CP-rich domains. This unique nanophase structure was a thermodynamically favored state as a delicate balance between the miscibility and self-aggregability of the CP and PVA chains in the glycerol medium, driven by hydrogen bonds and π-π interaction. On the one hand, both PVA and CP chains were prone to self-assemble themselves solely especially after thermal annealing at 80°C (Fig. 2g and Supplementary Fig. 21). The thermal annealing could significantly activate the segmental motion of PVA and CP by partially dissociating the hydrogen bonds (Fig. 2h and Supplementary Fig. 22), leading to more ordered molecular configurations as revealed by X-ray diffraction (XRD) spectra of PVA and Raman spectra of CP (Fig. 2i and Supplementary Fig. 23). On the others, the PVA and PSS chains in CP could strongly interact with each other through ionic hydrogen bonds, according to dynamic light scattering (DLS) spectra, Fourier-transform infrared (FT-IR), XRD spectra and mechanical tests (Fig. 2j, Supplementary Figs. 24–28, Supplementary Table 4). Furthermore, the glycerol, serving as an effective plasticizer through multiple hydrogen-bond interactions with both PVA and CP, could greatly suppress dense self-aggregation and thus enhance the polymer miscibility (Supplementary Fig. 29)24.

With the synergy of the two opposite tendencies as mentioned above, phase separation on the nanometer scale, therefore, occurred within the PVA-CP organogels, leading to the formation of a bicontinuous phase structure composed of PVA- and CP-rich domains. In detail, after thermal annealing, the CP-PVA organogels exhibited an improved degree of nanophase separation as shown by a significantly decreased interphase distance with high contrast in the phase images according to atomic force microscopy (AFM) characterizations (Fig. 2k). The nanophase separation structure could greatly benefit the electrical interconnection of CP chains while preventing their over-aggregation, thus leading to a uniform conductive percolation network throughout the PVA matrix. Additionally, the phase separation degree was quantified by small-angle X-ray scattering (SAXS). In SAXS, the scattering peak of PVA-CP organogels turned more pronounced with a positive shift after thermal annealing, corresponding to a decrease in the average interphase distance from 10.6 to 8.2 nm (Supplementary Fig. 30).

Worthy to note, the bicontinuous nanophase was thermodynamically favored in the glycerol medium and could be regulated by altering the chain mobility and intermolecular interaction (this will be discussed in the following). As a whole, driven by the hydrogen bonds, π-π stacking, and hydrophobic interaction, a delicate balance between the miscibility and self-aggregability of the CP and PVA chains was realized, thus leading to a bicontinuous nanophase structure composed of PVA- and CP-rich domains, where the former accounts for mechanical performance and the latter is responsible for electrical performance. The phase separation on the nanoscale could ensure the uniform distribution of conductive percolation networks and stress transfer pathways, thus rendering a successful integration of excellent electrical and mechanical performances (toughness).

Regulable conductance through the specific ion effect
Given that it is bicontinuous nanophases accounting for the successful decoupling of electrical and mechanical performance, the CP-PVA organogels’ conductance was therefore expected to be regulable if the nanophase structure could be engineered on demand. Herein, this hypothesis was successfully verified by introducing the specific ion effect into the organogel system. Specific ion effects, encompassing the Hofmeister series, originally describe a persistent trend in the effect of ions on the secondary structure and dispersibility of bio-macromolecules21. In general, cations with high charge density or anions with low charge density usually lead to higher solvation degrees of bio-macromolecules, while cations with low charge density or anions with high charge density often induce opposite effects. A widely accepted mechanism behind this phenomenon involves the ions impacting the solvation shell of molecules by electrostatic and polarization effects25. This phenomenon has also been extended to hydrogel systems recently, with examples including PVA26, polyampholyte27, and poly(N-isopropylacrylamide) (PNIPAm) hydrogels28. These hydrogels exhibited regulable mechanical properties (e.g., Young’s modulus) depending on the types of ions introduced into the system29.

For the CP-PVA organogels developed here, their conductance showed a high dependency on the types of ions introduced. Overall, cations showed a pronounced impact on the conductance of the organogels, following a similar ranking to the traditional Hofmeister series, whilst anions imposed a weak influence (Fig. 3a, b). Particularly, after being subject to treatment with glycerol solution containing 2 mol L−1 CaCl2 for 3 days (followed by selective evaporation at an ambient environment to evaporate most of the water), the CP-PVA conductive organogels transformed from a high-conductance state (27.3 S cm−1) (denoted as State I) to a high-resistance state (1.9 × 10−2 S cm−1) (denoted as State II) (Fig. 3c and Supplementary Fig. 31). This transition also reduced the Young’s modulus and toughness by 62 and 30%, respectively, with a slight change in solid content (51–44 wt%; Supplementary Fig. 32). Furthermore, the resistance of State II was maintained or even further increased by dialyzing out Ca2+ ion with glycerol solution, followed by selective evaporation at an ambient environment, to produce State III (residual Ca2+ ion content: ~0.5% relative to the carbon, Supplementary Figs. 31, 33 and Supplementary Table 5). In this state, the conductivity decreased to 3.3 × 10−3 S cm−1, while the mechanical performance and solid content remained stable. Moreover, State III could be reverted to the original high-conductance state by thermal annealing at 80°C for 2 h (State I), recovering the initial electrical and mechanical performance (Supplementary Figs. 31, 32). Therefore, this process established a closed regulatory cycle with a high conductance on/off ratio (defined as the conductivity ratio of State I to State III). Furthermore, this cycle could be repeated several times with no significant alteration in the electrical performance (Supplementary Fig. 34).

Mechanism and generality of nanophase reconfiguration
Such excellent adjustability of conductance could be ascribed to the reversible swinging of the nanophase structure within the CP-PVA organogels in three different thermodynamic states, highly distinct from previously reported cases in which conductance reconfiguration of gels commonly relied on swelling/deswelling of the system30 (Fig. 3d). In detail, firstly, the organogel in State I exhibited a bicontinuous phase structure as discussed in the above section, and should be thermodynamically favored given that thermal annealing was applied. Secondly, for State II, the bi-continuous phase was erased through Ca2+ treatment driven by thermodynamics. In detail, despite the Ca2+ could induce ionic crosslinking among partial PSS chains (Supplementary Fig. 35), these kosmotropic cations simultaneously interact with PVA chains, breaking the hydrogen bonds among them, as confirmed by FT-IR, XRD, and SAXS spectra (Fig. 3e and Supplementary Figs. 36, 37)29. The decrosslinking effect predominated over the ionic crosslinking, thereby enhancing the immiscibility of PVA and CP chains. As a result, the bi-continuous phase structure within the organogels was transformed into a more homogenous phase structure, leading to a highly resistive State II in the CP-PVA organogels. It is worth noting that such transformation should not be ascribed to the swelling of organogels, as no significant change in organogels’ solid contents was observed (selective evaporation at an ambient environment were implemented to evaporate most of the water absorbed during salt treatment before resistance measurement) (Supplementary Fig. 31). Moreover, the State II was also thermodynamically favored, as proved by the negligible change in resistance of the organogel containing CaCl2 after being subjected to thermal annealing at a high temperature of 60°C for 5 h (Supplementary Fig. 38). In addition, according to X-ray photoelectron spectroscopy, approximately 25% of PSS was removed during CaCl2 treatment in the first cycle, further supporting that nanophase structural was the primary factors governing the electrical properties, rather than compositional variations (Supplementary Fig. 39).

Thirdly, unlike the thermodynamically stable States I and II, State III was thermodynamically unstable but kinetically stable. The CP-PVA organogels after dialysis could remain highly resistant for a long duration at room temperature (e.g., 25°C for more than 7 days) (Fig. 3f). Such good kinetic stability could be attributed to the low chain mobility seriously retarded by hydrogen bonds among PVA and PSS chains. Subsequently, because of its thermodynamic instability, the organogel without CaCl2 could be transformed back to a high conductance state (State I) through thermal annealing at a high temperature of 80°C for 2 h, accompanied by the recovery of bicontinuous structure, as proved by AFM images, SAXS, and XRD spectra (Fig. 3e, g, and Supplementary Fig. 37).

Therefore, by harnessing the specific ion effect on the dynamic non-covalent interactions among polymer chains, reversible control over the organogels’ conductance with a high on-off ratio was successfully achieved. To further validate this mechanism, three sets of control samples were prepared, including CP-PVA organogels with varying CP contents or solid contents, CP-PVA hydrogels or organogels derived from other organic solvents, and chemically crosslinkable CP-PVA organogels (PVA-MA : methacrylate modified PVA) (Supplementary Figs. 40–53). The detailed discussion is provided in Supplementary Note 6. In brief, the control experiments further proved that the electrical reconfigurability originated from the dynamic response of polymers. Specially, organogels remained high on/off ratios of 103-104 across a wider range of CP content, but the ratio declined markedly at high loadings beyond a critical threshold of 34 wt% (Fig. 3h). Moreover, the conductance on/off ratios strongly correlated with the plasticization ability of dispersion media (solvent) in the organogels, specifically the hydrogen-bond-related Hansen solubility parameter (δh). Solvents with higher δh, which could offer more hydroxy groups for interaction with PSS and PVA24, impart greater adaptability to the polymer network, thereby enhancing the electrical reconfigurability of corresponding organogels (Fig. 3i, Supplementary Figs. 51–53 and Supplementary Table 6). Notably, in contrast to the previously reported cases in pure PVA hydrogel system29, cations showed a significantly stronger influence on the CP-PVA organogels than that of anions, as discussed above. This abnormal phenomenon suggested that the negatively charged CP (PEDOT:PSS) probably inhibited the anion penetration through electrostatic repulsion.

At last, the proposed electrical reconfiguration strategy showed good generality across different grades of PEDOT:PSS, alternative conductive fillers, and mechanical matrices (Supplementary Note 7, Supplementary Figs. 54–56). For example, the conductance reconfiguration was successfully achieved in organogels incorporating PEDOT:PSS with varying PSS contents (PEDOT:PSS ratios ≤ 1:3) or employing other ion-sensitive mechanical components (e.g., polyacrylamide and PNIPAm). In addition, the conductance on/off ratios of CP-PVA organogels remained stable across a wide range of environmental humidity level, demonstrating the high reliability and reproducibility of their electrical reconfigurability (Supplementary Fig. 57). As a whole, reversible control over the conductance of organogels was successfully achieved through nanophase structure engineering, leveraging the thermodynamically-driven reversible transformation of dynamic polymer networks in various ionic environments.

Reconfigurable printing circuit board with robust interfaces
With the highly dynamic characteristic of phase structure, the PVA-CP organogels provided an ideal platform for neuron-like bionic circuitry with remarkable reconfigurability at the hardware level, surpassing the limitations of previously reported intact conductive hydrogels or organogels. To showcase this unique feature, Rec-PCBs were fabricated by selectively annealing pristine CP-PVA organogels via laser irradiation, enabling the in-situ formation of patternable conductive domains through photothermal conversion (Fig. 4a).

To optimize the fabrication conditions, we first investigated the influence of the laser power on the conductivity and structural stability of CP-PVA organogels (Fig. 4b and Supplementary Fig. 58). With the laser power increasing (50-400 W m−2), all the CP-PVA organogels with varied CP’s and solid contents exhibited a similar conductivity trend: an initial increase with peak conductivities in a range of 4.5 S cm−1–107.1 S cm−1 at a laser power of 150 W m−2 (corresponding to a local temperature of ~85°C), followed by a decline at higher power. This reduction at relatively elevated power was likely due to the thermal-induced deswelling of organogels, as confirmed by infrared thermography (IRT) images and mechanical tensile tests, which showed localized overheating (e.g., ~200°C for 250 W·m−2) and deteriorated mechanical performance (Supplementary Figs. 58–60). Based on these results, a laser power of 150 W m−2 was identified as an optimum condition for the patterning of conductive pathways, using CP-PVA organogels with a solid content of ~50 wt% (relative to the total mass of organogels) and CP’s content of 22 wt% (relative to the total mass of CP and PVA) as the workpiece.

Upon laser irradiation, electrical circuits could be fabricated in situ within one CP-PVA organogel. The locally transformed conductive pathway, generated at a laser power of 150 W m−2, exhibited a low optical contrast to the naked eye, but with boundaries visible under backlighting conditions due to the slight dehydration under irradiation (Supplementary Fig. 59). To quantitatively study the photothermal-induced formation of conductive pathways, CP-PVA organogels were subject to laser irradiation through a photomask. First, all the conductive traces with linewidths ranging from 50 to 200 μm showed conductivities comparable to that of corresponding bulky materials, indicating the good size scalability of the laser-induced patterning (Supplementary Fig. 61). Second, the spatial resolution of the micropatterning process was evaluated by laser-writing pairs of adjacent conductive traces (Fig. 4c, d, and Supplementary Figs. 62, 63). Restrained by the inevitable thermal diffusion and resolution limit of the photomask used here, the minimum inter-line spacing between two conductive traces to avoid electrical cross-talk was determined to be 100 μm. Below this threshold, adjacent conductive traces became partially electrically connected. The resolution was expected to further improve by downsizing the laser spot through optical engineering in the future. Thirdly, the laser-induced conductive traces exhibited good uniformity and homogeneity in both horizontal and vertical directions: the absolute resistance of conductive traces followed Ohm’s law as shown by a good linear relationship with the trace length (Fig. 4e–g), and exhibited good consistency for both the upper (directly exposed to laser) and lower surfaces (Supplementary Figs. 64 and 65).

Moreover, distinct from the conventional circuit with fixed trace layout determined fabrication, the CP-PVA organogels developed here possessed remarkable dynamic characteristics, enabled by the reconfigurable nanophase structure, resembling the adaptive nature of biological neuron networks. To showcase this characteristic, a Rec-PCB model with an array of dumbbell-shaped conductive traces was fabricated by selectively irradiating a CP-PVA organogel. The conductance between pairs of contact pads in the array (Fig. 4h and Supplementary Fig. 66) was measured and found to lie in line with the traces of laser irradiation, where the patterned traces exhibited conductance values up to 3–4 orders of magnitude higher than those of not-irradiated regions. Moreover, the conductive pathway could be erased by CaCl2 treatment (followed by dialysis), resulting in a sharp resistance increase of 3–4 orders of magnitude. The pathways could then be rewritten through subsequent laser irradiation (Fig. 4i). This erasing-rewrite procedure could be repeated for more than 5 cycles, indicating the excellent reconfigurability (Supplementary Fig. 67).

In addition to enabling high reconfigurability, the in situ laser-assisted fabrication strategy also ensured the formation of a robust interface between the conductive traces and the surrounding matrix, attributed to the thermal gradient zone arising from inevitable heat diffusion within the organogels during irradiation (Fig. 4j). AFM analysis confirmed the presence of an interface layer between conductive and non-conductive domains. This layer facilitated remarkable interfacial adhesion and structural integrity through chain entanglement and non-covalent interactions (hydrogen bonds, π-π interactions, etc.) (Fig. 4k, l). The interfacial stability was successfully proved by tensile testing of CP-PVA organogels that were partially laser irradiated (Fig. 4m and Supplementary Fig. 68). The laser-patterned organogels showed mechanical performance comparable to that of pristine samples, with crack propagation formed upon strain commonly initiating at a random position rather than at the interface between irradiated and non-irradiated areas (Supplementary Video 1). Meanwhile, the patterned traces maintained stable electrical response under cyclic tensile strain, with no noticeable interfacial delamination (Supplementary Fig. 69). In contrast, most previously reported gel-based circuits lack in situ patternability and reconfigurability, and usually have to rely on adhesives for structural integrity.

Conformal soldering and closed-loop recycling
Beyond their electrical versatility, the high reconfigurability of CP-PVA organogels also enabled conformal soldering and closed-loop recyclability, advancing their utility in 3-dimensional (3D) and sustainable electronics. A widely used approach for the soldering of conductive gels involved a drying-reswelling procedure, where the conductive gels were dehydrated to achieve imitate contact with targeted substrates17. However, this strategy led to severe deformation or collapse of gels with complex 3D geometries. Herein, leveraging the high reconfigurability of the CP-PVA organogels, a geometry-preserving soldering strategy was developed to achieve strong and shape-retentive bonding between CP-PVA organogels and various substrates, without the need for complete dehydration.

In detail, for soldering, CP-PVA organogels at State III were coated with a thin layer of sans-glycerol CP/PVA aqueous solution (mass loading: 10 μL cm−2), gently pressed against the targeted adherend (5 kPa), selectively dried overnight (for mechanical bonding), and then thermally annealed at 80°C (for electrical connection). With this method, broken CP-PVA organogels could be healed together with no noticeable deterioration in mechanical and electrical performance (Fig. 5a–c). Importantly, complex geometries such as Möbius band structure could be preserved after soldering (Fig. 5d). In addition, CP-PVA organogels could also be strongly bonded to Cu, Sn, and Au substrates, achieving high adhesion toughness values of 1295, 1051, and 660 J m−2, respectively (Fig. 5e–g and Supplementary Figs. 70–72). The electrical contacts between CP-PVA organogel and metals were proved to be ohmic contacts as indicated by the linear current-voltage response (Supplementary Fig. 73). Furthermore, the electrical contact could also be spatially patterned by leveraging local laser irradiation, where only the irradiated domains were electrically connected. This method allowed for a multichannel board-to-board connection between CP-PVA organogel and flexible PCB (Fig. 5h), a capability not easily achieved with previously reported adhesion strategies23.

The mechanism underlying the wet soldering capability involved the solvent-mediated dynamic reconfiguration of the CP-PVA organogel network in the presence of the aqueous solder (sans-glycerol CP/PVA solution, Fig. 5i). Specifically, when aqueous CP/PVA solder was applied to the CP-PVA organogel at State III, the glycerol within the organogel and water from the solder underwent diffusion driven by a concentration gradient. On one hand, water infiltration partially loosened the original polymer network of organogels, resulting into a semi-interpenetrated network at the interface (Supplementary Figs. 74, 75a). Meanwhile, the glycerol in the organogels diffused into the aqueous solder and then induced the configuration transformation of CP (from solder) under thermal annealing (80°C) or local laser irradiation, thus reducing the contact resistance between CP-PVA organogels and substrates (Supplementary Fig. 75b). This mechanism was further supported by control experiments using solders with different components, including PVA/CP glycerol solution, sans-glycerol CP aqueous solution, and sans-glycerol PVA aqueous solution, which was detailed in the Supporting Information (Supplementary Note 8, Supplementary Fig. 76).

In the closed-loop recycling, the CP-PVA organogels could be reprocessed in a closed-loop route, enabled by the highly dynamic organogel networks and the low volatility of glycerol. In detail, through dialysis with minimal water to remove glycerol (the glycerol-containing solution was retained for reuse), the CP-PVA organogels could be well dissolved in water by heating at 80°C for 2 h (Fig. 5j). The resulting dispersion displayed excellent colloidal stability, with a zeta potential of −55 mV and uniform size distribution (295 nm), closing matching the original (−50 mV, 255 nm; Supplementary Fig. 77). Subsequently, new organogels could be regenerated by re-introducing the recovered glycerol solution (obtained in the dialysis process), drop-casting, and selective evaporation at ambient environments. The regenerated organogels exhibited only mild reduction in mechanical performance and electrical properties (e.g., 16.5 and 9.0% decreases in Young’s modulus and toughness, respectively; Supplementary Fig. 78). In addition, the regenerated organogels also inherited excellent electrical reconfigurability, in which the conductive pathway could be erased via CaCl2 treatment and then be re-constructed through laser scribing (Supplementary Figs. 79 and 80).

Demonstrations
As a whole, by in situ tuning of the nanophase structure of conductive organogels through specific ion effect, three pairs of inherently conflicted properties were successfully integrated within one system: (i) high electrical and mechanical performance, (ii) patternability and reconfigurability of highly conductive pathways, and (iii) in situ solderability and closed-loop recyclability of conductive gels. To showcase these capabilities, four representative applications were developed, including (i) organogel-based printing circuit boards (PCBs) for plug-and-play interconnection with conventional rigid PCBs, (ii) organogel-based integrated electronic wristbands for electrophysiological signal capture, (iii) in situ rewritable electroluminescent devices and rewritable LED bands, and (iv) organogel-based stretchable circuitry models for audio playing.

As a first example, a 6-channel organogel-based PCB was fabricated (line spacing: 5.5 mm, linewidth: 1 mm) (Fig. 6a). The PCB was soft, stretchable, and could be connected to conventional rigid PCBs through zero-insertion-force (ZIF) connectors for analog signal transmission (Fig. 6b). Attributed to the high structural integrity with high toughness, the electrical connection/disconnection of organogel-based PCB to the conventional rigid PCB could be repeated for >1000 cycles, with no noticeable deterioration in electrical performance (Supplementary Fig. 81). Moreover, the organogel-based PCB demonstrated a broader operational frequency range compared to its hydrogel counterpart, probably due to the lower relative permittivity of the organic system (Supplementary Fig. 82).

Secondly, a CP-PVA organogel-based digital wristband in situ patterned with 8 pairs of electrodes was prepared for electrophysiological signal recording (Fig. 6c). In detail, the good biocompatibility of CP-PVA organogels was a prerequisite for high-quality signal acquisition, which was confirmed by both in vitro cytocompatibility tests and in vivo subcutaneous implantation assessment (Supplementary Note 9, Supplementary Fig. 83)31,32. Furthermore, compared to the previously reported bioelectrodes, the digital wristband showed low electrical impedance and robust structural integrity while maintaining a stable electrical connection when interfaced with a signal recorder via a PCB through a conformal soldering method as described above (Fig. 6c, Supplementary Figs. 84, 85)33. Particularly, the overall impedance and phase angle of the digital wristband exhibited negligible changes under 50% tensile stretching, demonstrating the excellent reliability of the system (Supplementary Fig. 86). Consequently, high signal-to-noise ratio electrophysiological recordings were achieved, surpassing those obtained with commercially available electrodes (Supplementary Fig. 87). As an example, real-time monitoring of muscle activity was demonstrated by recording the surface electromyography (sEMG) maps in space and time domains, highlighting potential applications in medical diagnosis or human-machine interaction (Fig. 6d, e, Supplementary Fig. 88 and Supplementary Video 2). At last, the CP-PVA organogel-based digital wristband demonstrated excellent environmental stability, maintaining a high signal-to-noise ratio (~21 dB) and reliable sEMG recording performance even after one week of exposure to ~20% and ~70% relative humidity conditions (Supplementary Fig. 89).

Thirdly, to showcase the reconfigurability, organogel-based electroluminescence (EL) devices and rewritable LED bands were prepared (Fig. 6f, g, Supplementary Figs. 90, 91). The EL devices consisted of a laser-patterned PVA-CP bottom electrode, polydimethylsiloxane (PDMS)-ZnS EL layer, and Cu top electrodes. Upon electric power, the EL emission accurately replicated the layout of the electrical traces patterned within the CP-PVA organogels. More importantly, the layout could be dynamically altered by in situ rewriting the conductive traces through sequential treatment with CaCl2 solution, dialysis, and laser scribing (Fig. 6f, Supplementary Figs. 92, 93, and Supplementary Video 3). The reconfigurable LED band featured an LED matrix soldered onto the CP-PVA organogel substrate using PVA/CP aqueous solder. Its conductive pathways could be adjusted by leveraging the electrical reconfigurability of CP-PVA organogel, enabling on-demand modification of the electrical layout (Fig. 6g, Supplementary Fig. 91).

Notably, beyond these examples, the hardware-level reconfigurability is expected to inspire the design of next-generation biomimetic electronics for a variety of applications, including tissue engineering, information processing, and cyborgs. For example, dynamically reconfigurable conductive organogels could support neural tissue culture with spatiotemporal plasticity.

Finally, to demonstrate the excellent solderability of the CP-PVA organogels for use as printing circuit boards, a functional stretchable audio-playing circuit was assembled. The circuit comprised resistors, capacitors, switches, an LED, a speaker, and an FLM038A integrated circuit (IC) (Fig. 6h, Supplementary Fig. 94, Supplementary Table 7). The electronic components were soldered onto a laser-patterned organogel-based PCB using CP/PVA aqueous solder followed by thermal annealing, resulting in strong bonding and reliable electrical connectivity. The final circuit was highly soft, stretchable, and capable of playing preloaded audio tracks stored in the FLM038A chip during operation (Supplementary Video 4). At last, given the ion-specific mechanism that underlies the organogel’s phase reconfigurability, the CP-PVA organogel-based circuit board was expected to be sensitive to ions, especially kosmotropic cations. A potential strategy to mitigate this issue involves encapsulating the organogels with detachable ion-selective barrier materials after fabrication, which will be explored in future studies.

Methods
Materials
Poly(3,4-ethylenedioxythiophene):polystyrenesulfonate was ordered from Heraeus Epurio Ltd (Grade PH1000) or Sigma-Aldrich (Orgacon™ ICP 1050), or prepared following the method described below. Glycerin (AR, 99%), Acrylamide (AR, 99%), ammonium persulphate (APS, AR, 98%), methacrylic anhydride were (94%, Contains 2% stabilizer), triethylamine (AR, 99%), and α-Ketoglutaric acid (98%) were supported by Haohong Pharmaceutical Co., Ltd. (Shanghai, China). Poly(vinyl alcohol) (PVA, Mw: 89000–98000, 99% alcoholysis), aniline (AR, 99%), silver powder (Ag, 5 μm), sodium chloride (NaCl, 98%), potassium chloride (KCl, 98%), cesium chloride (CsCl, 98%), lithium chloride (LiCl, 98%), calcium chloride (CaCl2, 98%), sodium sulfate (Na2SO4, 98%), sodium carbonate (Na2CO3, 98%), sodium citrate (98%), sodium iodide (NaI, 98%), acetone (98%), ethanol (98%), hydrochloric acid (HCl, analytical reagent grade), and dimethyl sulfoxide (DMSO) were purchased from Shanghai Aladdin Biochemical Technology Co., Ltd.

Synthesis of PEDOT:PSS with varying PSS contents
PEDOT:PSS was synthesized via oxidative polymerization of 3,4-ethylenedioxythiophene (EDOT) in the presence of sodium polystyrene sulfonate (NaPSS, Mw: ~20kDa). Briefly, EDOT monomer (50 μL, 47 mmol) was dispersed in 15 mL of NaPSS aqueous solution under vigorous stirring at room temperature, with the molar ratio of EDOT to the sulfonate units of NaPSS adjusted to be 1:3, 1:4, or 1:5. The mixture was stirred for 30 min to ensure uniform dispersion and effective interaction between EDOT and NaPSS. Subsequently, anhydrous ferric chloride (FeCl3, 15.3 mg) and sodium persulfate (130 mg, 55 mmol) were added, and the reaction was allowed to proceed under continuous stirring for 12 h. During this period, the solution gradually turned dark blue, confirming the formation of PEDOT:PSS. Finally, the resulting dispersion was purified using cation- and anion-exchange resin to remove residual salts.

Preparation of CP-PVA organogels
Typically, unless otherwise specified, PEDOT:PSS aqueous solutions with the grade of PH1000 from Heraeus Epurio Ltd were used for the preparation of CP-PVA organogels. This PEDOT:PSS grade was one of the most widely used formulations in the research community, attributed to its high conductivity and excellent processability. The pristine PEDOT:PSS aqueous solutions were first filtered through a syringe filter with a pore size of 0.45 μm to remove large particles and then added to a PVA glycerol solution (the content of glycerol was 4 wt% relative to the total mass of final solution, and the concentrations of CP and PVA were 7.4 mg mL−1 and 26.1 mg mL−1 respectively, if not particularly mentioned). The obtained suspension was drop-casted on a glass plate (volumetric loading: 0.1 mL cm−2) and dried at the ambient environment (~25°C) overnight to obtain free-standing p-CP-PVA organogels with a thickness of ~92 μm. The solid contents of p-CP-PVA organogels could be controlled by varying the glycerol’s relative contents in the precursor solutions. The p-CP-PVA organogel exhibited a high resistance. To improve the conductance, a dry annealing process was implemented at 80°C for 2 h at ambient conditions with relative humidity (RH) of 40–60%.

For the preparation of a thin CP-PVA organogel film with high optical transparency, a spin-coating method was employed, where the precursor glycerol solutions containing CP and PVA were spin-coated onto glass plates or elastomer films (EcoflexTM 00-45 Near ClearTM) previously treated by oxygen plasma at speeds of 500, 700, 900, 1100, 1300, and 1500 rpm. At last, conductive organogel film was obtained by drying at the ambient environment (~25°C) overnight and an annealing process at 80°C for 2 h.

In the control experiments, four types of samples were prepared, including CP-PVA organogels based on other organic solvents, CP-PVA hydrogel, pure CP, and PVA organogels. (i) CP-PVA organogels based on other organic solvents: different solvents (DMF, DMSO, ethylene glycol, and polyglycerol, respectively) were added into the CP-PVA mixture solution (mass ratio of CP to PVA=22:78), and organogels were obtained following a similar procedure as described above. (ii) CP-PVA hydrogels: CP-PVA organogels were dialyzed in water, dried at the ambient environment (25°C, ~50 % relative humidity), and then reswollen in deionized water to yield CP-PVA hydrogels. (iii) Pure CP organogels: PEDOT:PSS suspensions were added with glycerol (4 wt%, relative to the total mass of solution), and then drop-casted onto glass plates previously treated with O2 plasma for 5 min (volumetric loading: 75 μL cm−2), followed by annealing at 80°C for 2 h. (iv) Pure PVA organogels: PVA glycerol suspensions containing 4 wt% glycerol and 10 wt% PVA were drop-casted onto glass plates previously treated with O2 plasma for 5 min (volumetric loading: 30 μL cm−2), and dry annealed at 80°C for 2 h.

Preparation of methacrylate PVA (PVAMA) and CP-PVAMA organogels
The PVAMA was synthesized by the esterification reaction between PVA and methacrylic anhydride, following the previous literarure34. First, PVA (Sigma-Aldrich, 89000–98000 kDa, 98% hydrolyzed) was dissolved in water by heating at 90°C for 2 h to obtain a 10 wt% PVA solution. Then, the PVA solution was added with methacrylic anhydride (5 mol% relative to PVA) under stirring, left to react at 60°C for 48 h, and then quenched by neutralizing with triethylamine. At last, PVA-MA power was obtained by slowly dropping the reaction solution into acetone (5 equivalent volumes relative to the solution) under vigorous agitation, filtering, washing with excessive acetone, and drying at 60°C.

For the preparation of the CP-PVAMA organogels, glycerol suspensions (4 wt%, relative to the total mass of solution) containing 7.4 mg mL−1 of CP, 0.3 mg mL−1 of α-ketoglutaric acid, and 26.1 mg mL−1 of PVAMA (CP’s relative content: 22 wt%) was dropped-casting on a glass plate (volumetric loading: 0.1 mL cm−2), and dried under ambient conditions (25°C) for 24 h to selectively evaporate most of the water. At last, a free-standing CP-PVAMA organogel was successfully obtained and crosslinked by exposure to ultraviolet (UV) light (wavelength: 365 nm) for 30 min. For the preparation of CP-PVAMA organogels without chemical crosslinking, a polymerization inhibitor was added to a sans-photoinitiator glycerol solution (4 wt%, relative to the total mass of solution) containing 7.4 mg mL−1 of CP and 26.1 mg mL−1 of PVAMA (CP’s relative content: 22 wt%, relative to the total mass of PVAMA and CP), and then followed with a similar procedure as described above except without UV exposure step.

Preparation of polyaniline (PANi)-PVA and Ag-PVA organogels
PANi-PVA organogels were synthesized following an ice-templated polymerization method reported previously35. In detail, a monomer-containing solution (solution A) was first prepared by adding 80 μL of HCl solution (35 wt%) and 28 mg of aniline in 1 mL of 10 wt% PVA solution, followed by vigorous stirring until a clear and transparent solution was formed. The mixture solution was cooled in an ice bath. Subsequently, 0.5 mL of ammonium persulfate (APS) solution (162 mg mL−1) was added to solution A. The resulting solution was poured into a mold and frozen in liquid nitrogen for 2 h. Finally, the frozen samples were transferred to a refrigerator at −20°C and kept static for 24 h, during which aniline was polymerized to form PANi. PANi-PVA organogels were obtained by thawing the frozen samples at room temperature, followed by dialysis in 50 wt% glycerol solution for 12 h and drying at ambient temperature for 24 h.

For the preparation of the Ag-PVA organogels, 0.15 g of silver flake powder (diameter: 5 μm) and 0.6 mL of a glycerol solution (50 wt%) were added to 2 mL of a 10 wt% PVA solution and mixed with a planetary-type mixer at 2500 rpm for 10 min (HMV200D, Shenzheng Hasai Technology, China). Then, the mixture solution was drop-casted onto a glass plate (volumetric loading: 0.1 mL cm−2) and dried at ambient temperature (~25°C) for 24 h.

Preparation of CP-PAM organogels and CP-PNIPAm organogels
PAM was first synthesized by free radical polymerization in aqueous solution. Specifically, 1.0 g of acrylamide monomer was dissolved in 10 mL of deionized water to obtain a clear 10 wt% solution. Ammonium persulfate (APS, 10 mg, corresponding to 1 wt% of acrylamide) was then introduced as the radical initiator, followed by the addition of tetramethylethylenediamine (TEMED, 5 μL, ~0.5 wt%) as the accelerator. The solution was purged with nitrogen for 20 min to remove dissolved oxygen, sealed, and allowed to polymerize at ambient temperature (25°C) under gentle stirring for 4 h. The viscous product was dialyzed against deionized water for 48 h to remove unreacted monomers and initiators, and subsequently freeze-dried to obtain linear PAM in the form of a white powder. For CP-PAM organogel preparation, pristine PEDOT:PSS aqueous solution was first passed through a 0.45 μm syringe filter to remove large particles. The filtered PEDOT:PSS was then mixed with a PAM–glycerol solution, in which glycerol accounted for 4 wt% of the total solution, while the concentrations of CP and PAM were maintained at 7.4 mg mL−1 and 26.1 mg mL−1, respectively (unless otherwise specified). The resulting suspension was drop-cast onto a glass plate with a volumetric loading of 0.1 mL cm−2 and dried overnight at ambient conditions (~25°C) to yield free-standing p-CP-PAM organogels. The as-prepared organogels initially exhibited high resistance, which was subsequently reduced by subjecting the samples to a thermal annealing treatment at 80°C for 2 h to improve their electrical conductivity. CP-PNIPAm organogels were synthesized using a similar procedure, with PNIPAm replacing PAM as the polymer matrix.

Transitioning of CP-PVA organogels among different conductance states
Unless otherwise specified, the CP-PVA organogels used in the tests had a solid content of ~50 wt% (relative to the total mass of organogel) and a CP fraction of 22 wt% (relative to the total mass of CP and PVA). (i) The thermally-annealed CP-PVA organogels were donated as State I. (ii) To obtain State II, the CP-PVA organogels in State I were soaked with a glycerol solution containing 2 mol L−1 CaCl2 for 3 days, followed by selective evaporation at an ambient environment (~25°C, RH: 40–60%) for 24 h. (iii) To obtain State III, the CP-PVA organogels at State II were dialyzed in a 15 wt% glycerol solution for 24 h and partially dried in an ambient environment for 24 h. (iv) To obtain State I, the CP-PVA organogels at State III were thermal annealed at 80°C for 2 h under ambient conditions (~25°C, RH: 40–60%).

To pattern the conductive traces, the p-CP-PVA organogels or CP-PVA organogels at State III were irradiated by a continuous laser (DT1-3W; Lighthouse Photonics, China) with an optical power density of 150 W m−2 (wavelength: 532 nm, spot size: 0.3 mm) at a fixed scanning speed of 6 cm s−1, if not mentioned. An infrared thermal imager (A615, Teledyne FLIR, U.S.) was employed to record the temperature variations and infrared thermal images of the CP-PVA organogels during laser irradiation, capturing their photothermal response. To obtain fine conductive traces, CP-PVA organogels at State III were subject to laser irradiation through a photomask. The pre-patterned photomask was brought into intimate contact with the organogel surface and precisely aligned under microscopic observation (the design of the photomask is shown in Supplementary Figs. 61, 65). Laser irradiation was subsequently applied through the photomask apertures to induce conductive traces. To erase the conductance of the CP-PVA organogels, the CaCl2 treatment and dialysis were performed, following the protocol described above.

Determination of water and glycerol contents in organogels
The solid content of CP-PVA organogel was obtained by measuring the total mass (mt) of wet samples and dry mass (ms) after complete drying. To determine the glycrol contents, the dispersion medium of organogel was extracted by dialysis in a defined amount of deionized water (2 mL) and filtered through a membrane with a pore size of 0.22 μm prior to high-performance liquid chromatography (HPLC) analysis. The measurements were performed on an HPLC system (Waters e2695, Waters Corporation, US) equipped with a refractive index detector and an Aminex HPX-87H column (300 mm × 7.8 mm, 9 μm). The column temperature was set as 35°C, and 5 mmol L−1 H2SO4 was used as the mobile phase at a flow rate of 0.6 mL min−1. Standard glycerol solutions (0.02–1.0 mg mL⁻¹) were freshly prepared to construct an external calibration curve (linear correlation coefficient, R2≥0.999). The mass fractions of glycerol (Fg) and water (Fw) in the CP-PVA organogel were calculated using Eq. (1) and Eq. (2), respectively.

Fg= Cgly × 2mL / mt × 100% (1)

Fw= (mt − ms − Fg × mt) / mt × 100% (2)

where Cgly is the concentration determined from the calibration curve.

Conformal soldering of conductive organogels and measurement of contact resistance
The CP-PVA organogels could be soldered to themselves or some common metals such as Cu, Sn, and Au. Typically, CP-PVA organogel was first dip-coated with a sans-glycerol CP/PVA aqueous solution (containing 26.1 mg mL−1 PVA and 7.4 mg mL−1 CP) and then gently pressed against the targeted adherend (~5 kPa), and left to stand at an ambient temperature (~25°C) for 12 h. Afterward, the assembly was thermally annealed at 80°C for 2 h or subjected to via local laser irradiation to establish an electrical connection. Particularly, for bonding with metal substrates, the surface was first cleaned with ethanol to remove organic contaminants, followed by 5 min of oxygen plasma treatment to enhance surface hydrophilicity.

In the control experiments, different soldering solutions were employed including PVA/CP glycerol solution (glycerol content: 4 wt% relative to the total mass of the final solution, CP and PVA concentrations: 7.4 mg mL−1 and 26.1 mg mL−1 respectively), sans-glycerol aqueous CP solution (solid content: 1.1–1.3 wt%), and sans-glycerol aqueous PVA solution (solid content: ~10 wt%). The soldering process was then performed following the same procedures as described above.

The contact resistances between the organogel and conductive adherent were measured using a source meter (2450 Graphical Source Meter, Keithley, U.S.) in a two-probe configuration. A linear voltage sweeps from −3 V to +3 V were applied, and the corresponding current response was recorded.

Fabrication of organogel-based printing circuit boards
The CP-PVA organogels, with a solid content of ~50 wt% and CP’s relative content of 22 wt% (relative to the total mass of CP and PVA), were used for experiments. The CP-PVA organogels were cut into rectangular strips measuring 10 cm in length and 3.5 cm in width using a scalpel. Subsequently, 6 channels conductive traces (spacing: 5.5 mm, width: 1 mm) were induced on the CP-PVA organogels via continuous laser direct writing with an optical power density of 150 W m−2 (wavelength: 532 nm, spot size: 0.3 mm) at a fixed scanning speed of 6 cm s−1. The organogel-based printing circuit traces could be connected to two zero-insertion-force (ZIF) connectors, capable of transmitting analog signals within a wide range of frequencies (10 MHz-100 HZ).

Closed-loop recycling of conductive CP-PVA organogels
CP-PVA organogels can be closed-loop recycled through dissolution followed by selective solvent evaporation. Specifically, CP-PVA organogels (30 mm in length and 20 mm in width) with laser-patterned conductive traces were dialyzed in a small amount of water to remove glycerol, and the resulting dialysis solution containing glycerol was collected for subsequent reuse. The dialyzed sample was then dispersed in 1 mL of deionized water and stirred at 80°C until a clear solution was obtained. After cooling to room temperature, the previously collected dialysis solution was added to recover the glycerol content (2 wt%, relative to the total mass of the solution). The resulting mixture was filtered through a 220 μm pore size membrane, drop-cast onto a glass plate (volumetric loading: 0.2 mL cm⁻2), and allowed to dry under ambient conditions (25°C) for 24 h.

Preparation of organogel-based electronic wristband and EMG
An p-CP-PVA organogel (180 mm × 50 mm × 75 μm) was patterned into electrical traces by a continuous laser (150 W m−2, wavelength: 532 nm, spot size: 0.3 mm, speed: 6 cm min−1) to fabricate a one-body digital wristband. The resulting digital wristband was connected to a biosignal acquisition board (Cyton Board, OpenBCI, U.S.) via a flexible printed circuit board (FPCB) for EMG recording. The electrical connection between the wristband and the FPCB was achieved using the conformal soldering method described above, where an aqueous CP/PVA solder was applied at the interface and selectively irradiated by laser (Fig. 6c). The acquired signals were wirelessly transmitted to a computer via Bluetooth and post-processed with band-pass (0.5–100 Hz) and notch (50/60 Hz) filters.

Fabrication of in-situ rewritable electroluminescence devices
Organogel-based electroluminescence devices adopted a sandwich structure36, consisting of a patterned organogel bottom electrode, an electroluminescent layer, an insulating layer, and a Cu top electrode (Supplement Fig. 88). Patterned p-CP-PVA organogels (solid content: 40 wt%, relative to the total mass of organogels, CP content: 22 wt% relative to the total mass of CP and PVA), serving as the bottom electrode, were prepared through laser irradiation as described above. The patterned p-CP-PVA organogels were then coated with a ZnS electroluminescent layer through blade-coating uncured PDMS precursor containing ZnS particles (mass ratio of PDMS to ZnS = 1:1.4) and solidifying in the ambient environment (25°C) for 4 h. Next, barium powder was dispersed in uncured PDMS at a 1:1 mass ratio and applied atop the light-emitting layer to serve as the insulating layer, followed by curing in the ambient environment for 2 h. Finally, conductive copper paste was applied to the surface of the insulating layer to form the electrode layer. The EL devices were activated by applying an alternating current of 100 V and 3 kHz between the CP-PVA organogel and the conductive copper electrodes.

To reconfigure the electroluminescent pattern, a 15 wt% glycerol solution containing 2 M CaCl2 solution was dropped onto the surface of the bottom electrodes in the EL devices and left static for 3 days, during which the previously patterned conductive traces were erased (Supplementary Fig. 90, 91). Then, CaCl2 was removed by repeated dialysis in a 15 wt% glycerol solution (four times), followed by partial drying in the ambient environment. The recovered high-resistance organogel electrode was subsequently repatterned with new conductive traces via continuous laser direct writing, enabling the rewriting of the electroluminescent pattern.

Fabrication of in-situ rewritable LED bands
The p-CP-PVA organogels, with a solid content of ~40 wt% and CP’s relative content of 22 wt% (relative to the total mass of CP and PVA), were used for experiments. Subsequently, conductive traces were patterned on the CP-PVA organogel by a continuous wave laser (power density: 150 W m−2, wavelength: 532 nm, spot size: 0.3 mm, speed: 6 cm min−1). The conductive traces as shown in Supplementary Fig. 53. The aqueous CP/PVA solder (the concentrations of CP and PVA were 7.4 mg mL−1 of CP and 26.1 mg mL−1) was printed onto the CP-PVA organogel through a customized stencil, serving as contact pads for LEDs. Then, the LEDs are placed on the corresponding contact pads. Finally, the LED bands were left at ambient temperature (~25°C) to selectively evaporate excess water from the CP/PVA aqueous solder, and powered by a constant current of 20 mA.

To study the in-situ re-writability of CP-PVA organogel-based LED bands. CP-PVA organogel-based LED bands were immersed in 15 wt% glycerol solutions (relative to the total mass of solution) with a salting-in effect (e.g., 2 M CaCl2 solution) for 3 days. Then, the LED bands were dialyzed in 15 wt% glycerol solution for 24 h and selectively evaporated in an ambient environment (~25°C) overnight to erase the conductive traces of CP-PVA organogels. The CP-PVA organogels were subsequently rewritten with new conductive traces via continuous laser direct writing with an optical power density of 150 W m−2 (wavelength: 532 nm, spot size: 0.3 mm) at a fixed scanning speed of 6 cm s−1 (Supplementary Fig. 53).

Fabrication of organogel-based stretchable circuitry model for audio playing
The organogel-based stretchable circuitry model was fabricated by constructing an audio circuit with a patterned CP-PVA organogel serving as a printing circuit board. Here, we patterned the p-CP-PVA organogels to create conductive traces and contacts for circuit applications. The p-CP-PVA organogels, with a solid content of ~40 wt% and CP’s relative content of 22 wt% (relative to the total mass of CP and PVA), were used for experiments. Subsequently, conductive traces were constructed on the p-CP-PVA organogels by a continuous wave laser (power density: 150 W m−2, wavelength: 532 nm, spot size: 0.3 mm, speed: 6 cm min−1). The CP/PVA aqueous solder (the concentrations of CP and PVA were 7.4 mg mL−1 of CP and 26.1 mg mL−1) was printed onto the p-CP-PVA organogel, serving as contact pads for electronic components. The electronic components are placed on the corresponding contact pads. Finally, the electronic components were left at room temperature to allow the evaporation of excess water from the CP/PVA aqueous solder. Detailed circuit diagram and printed circuit board design are provided in Supplementary Fig. 54, and the list of components can be found in Supplementary Table 5. The organogel-based audio player circuit was powered by a lithium-ion battery.

Statistical analysis
All experiments were conducted with a sample size of at least four (n≥3), and results were presented as mean ± standard deviations (SD) or as box-and-whisker plots. Statistical analyses were performed using the two-sided t-test for comparisons between two groups or one-way analysis of variances (ANOVA) for comparison among multiple groups, using Origin software. Significance levels were assessed using p values. For AFM characterizations shown in Figs. 2k, 3g, and 4j–l, the displayed images correspond to one of the repeated trials, and the reproducibility across independent replicates was confirmed. Electrophysiological recording data were pre-processed using a bandpass filter (5–50 Hz) implemented in Origin software. All statistical analyses were performed using IBM SPSS Statistics 27.

Peer review rounds
[{"round": 1, "reviewer_comments": {"reviewer_1": "Zhong et al reported on \"Highly reconfigurable neuron-mimicking conductive networks through nanophase structure engineering\" This research introduces a novel strategy for developing next-generation bionic electronics by leveraging specific ion-mediated reversible nanophase reconfiguration within conductive organogels. The manuscript presents significant process in dynamic material engineering. However, there are critical concerns regarding the biomedical relevance and lack of physiological compatibility validation. To support ther claims, additional confirmation is needed, as outlined below. Hence, we opted for a minor revision of these findings.\n1.Lack of biocompatibility evaluation: the organogels developed in this work are intended for direct or semi-direct contact with biological tissue (e.g., skin-mounted digital wristbands for EMG recording). However, the manuscripts dose not present any biocompatibility assessment, such as cytocoxicity, hemocompatibility, or inflammation-related assays. Inclusion of in vitoro cell viability studies is strongly recommended to confirm safety for on-skin or in vivo use. We recommend referencing biocompatibility evaluation methods as demonstrated in “ Lubricant-infused Polymeric Interfaces: A stretchable and anto-fouling surface for implantable biomaterials (Adv. Funct. Mater. 2024)”, which provided a clear protocol for cell viability and cell aspect ratio analysis for biomedical application. Adoption similar in vitro testing methods would significantly support the climed biomedical applicability of th CP-PVA organogels.\n2.Mechanical mismatch with skin tissue: The reported Young’s modulus of 2.8-13.5 MPa exceeds that of soft biological tissue (typically 100-500 KPa for skin). For conformal applications, such a mechanical mismatch may result in poor adhesion, skin irritation, or mechanical fatigue. If for dermal interfacing, modulus adjustment strategies or design accommodations should be considered.\n3.Role of residual ions and skin exposure: the conductivity switching mechanism relies on CA2+ and other ions. However, the residual presence of these ions post-treatment (especially after CaCl2 exposer) is not clearly addressed. This raises concerns about ionic leaching, potential local toxicity, and electrolyte imbalance when interfaced with biological systems.\n4.For the EMG measurement section in Figure 6, it would be beneficial to include additional experimental data, if available. Supplementary materials, such as a real-time measurement video, could further enhance the manuscript. Additionally, more detailed information regarding the EMG measurement system is needed. Currently, only the electrodes are described, and there is limited discussion on how the system reliably captures such subtle biosignals. Considering the challenges of maintaining a high SNR at micro- to millivolt scales, and given that the PCB appears to serve as a simple rigid connector, further technical details about the measurement equipment and sensors would strengthen the manuscript.\n5.Further explanation of the erasing and rewriting process shown in Figure 6f would be helpful. The current supplementary video appears to focus on the formation of a QR code, but does not clearly demonstrate the rewriting process. Including either direct experimental evidence or an illustrative depiction of the rewriting process would provide greater clarity for readers.\n6.There are several instances throughout the manuscript where the arrangement of text and images within the figures appears misaligned. For example, in Figure 1c,d, some text overlaps with the images, and in Figure 3f, text seems to be misplaced, potentially leading to confusion about the figure content. Overall, the quality and clarity of the figures do not fully meet the standards expected for this journal, which makes it difficult to interpret the data. I recommend a thorough revision of all figures to ensure proper alignment, clear labeling, and improved overall presentation.", "reviewer_2": "This paper introduces a novel strategy for designing reconfigurable bioelectronic materials by using reversible nanophase regulation in dynamic, physically crosslinked conductive networks. The organogels —based on conducting polymers (PEDOT:PSS), polyvinyl alcohol and glycerol—exhibit both significant electrical conductivity and excellent mechanical properties thanks to a nanophase separation which can be disturbed and recovered through an treatment with kosmotropic cations Ca2+ (specific ion effect), dialysis and annealing. By this approach, fully characterized by numerous technics, the authors shows unique features such as micro-patternability, in situ solderability, recyclability, and global (annealing) or local (laser) control of the electronic conductivity. The proposed organogels show much better performances and stability that the corresponding hydrogels. This approach aims at mimicking the adaptability of biological tissues, offering a promising route toward advanced bionic electronics. By this original approach, the authors demonstrate that their system overcomes the classical trade-off between electrical conductivity and dynamic mechanical behavior, thanks to the ion-induced modulation of nanophase structure. They also show compatibility with rigid electronics (e.g., flexible PCB), which is a major challenge in gel-based bioelectronics. The authors push the effort to the generalization of their approach with first results on other materials (e.g., Ag, polyaniline).\nTo summarize my opinion, the paper is trully excellent and impressive, both from the amount and the quality of the results. The significance of the achievements is high and all conclusions are strongly supported by numerous and relevant characterizations but also by several very convincing demonstrations. I am sure that this paper will be of great interest for the community and I recommend its publication providing few minor revisions:\n- Could the authors elaborate on the choice of the PEDOT:PSS grade? It is simply stated “Poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS, solid content: ~1.1 wt%) was ordered from Heraeus Epurio Ltd” in the Materials section. Knowing that numerous grades, with various molecular weight or various ratio between PEDOT and PSS are available, does any grade would be compatiblewith the proposed? Is the chosen grade the classical “PH1000” commonly used by the community?\n- Please carefully check if all the information on composition are provided for each steps. Indeed, the various ratio investigated in the synthesis/characterization part of the manuscript makes it sometimes unclear which composition is chosen for subsequent experiments\n- In the section “Mechanism on the nanophase structure reconfiguration”, the authors state that “In detail, the kosmotropic cations Ca2+ could bind with PVA chains to break the hydrogen bonds among them”. There is no mention of a possible interaction between cations and the polyanionic PSS.\n- What happens to the content of PSS during the Ca2+ treatment/dialysis steps? In classical PEDOT:PSS systems, it is well-known that solvent annealing or washing can remove partly the insulating PSS, leading to an enhancement of conductivity. What happens in this present case? Can the author provide evidence of the removal or not-removal of the component which is initially present in a significant amount in the organogel?", "reviewer_3": "This manuscript introduces a strategy termed nanophase structure engineering to develop hydrogel materials with tunable conductivity, enabling subsequent device fabrication via laser engraving. The overall concept is clearly presented, and the experimental work is thorough. However, several concerns regarding novelty and mechanistic interpretation remain. In its current form, the work appears to be a combination of previously reported strategies without a sufficiently distinct innovation. The following comments outline key points that must be addressed to strengthen the manuscript’s contribution and justify its suitability for publication in Nature Communications.\nMajor Comments\n1. Many elements of the work closely resemble previously published studies: phase‐separation engineering (e.g., Nat. Mater. 22, 895–902 (2023)), solvent‐annealing to boost conductivity (e.g., Nat Commun 14, 2206 (2023)), the Hofmeister effect in conductive polymers (e.g., works from Xinmin He group), laser‐induced conductivity and adhesion in PEDOT hydrogels (e.g., Nat Electron 7, 475–486 (2024)), and conformal soldering techniques (Sci. Adv.10, eadp0730 (2024)). The authors should clarify what is fundamentally new in their approach, explicitly contrast it with these precedents.\n2. In the synthesis of pristine CP-PVA organogels, drying the mixture at ambient conditions for 24 h does not guarantee complete water removal because glycerol binds water via hydrogen bonding. Residual “bound” water may remain, and its amount will vary with the glycerol:water ratio, significantly affecting the hydrogel’s final properties.\n3. The claim of successfully decoupling conductivity and toughness is not fully supported by Figure 2a–d. The hydrogel reaches maximum toughness at 22 wt % CP (27.3 S cm⁻¹) but highest conductivity at 34 wt % CP (112.5 S cm⁻¹) with much lower toughness (<12 MJ m⁻³). Selecting the best values for each property under different conditions is misleading. Instead, report conductivity and toughness measured on the same sample batch or clearly explain why different compositions should be compared side by side.\n4. Given the critical role of annealing, the Methods section needs far more detail: Was annealing performed in a controlled‐humidity chamber (dry annealing) or in a solvent bath (wet annealing)? What temperature, duration, and atmosphere were used? Furthermore, both CP and glycerol contents change during annealing; please decouple the effects of compositional shifts from nanophase restructuring.\n5. The in-depth characterization focuses on CP–PVA interactions but largely overlooks the role of glycerol, which comprises a large fraction of the material and forms strong hydrogen bonds with PVA. Please discuss how glycerol influences nanophase formation and mechanical behavior. Additionally, since PEDOT:PSS contains both PEDOT and PSS, specify which moiety interacts with PVA while discussing.\n6. The authors demonstrate tunable conductivity via Hofmeister salts but do not report the corresponding mechanical properties. After ion‐specific treatment and re-annealing, are toughness or elasticity preserved compared to the untreated hydrogel? Please provide mechanical data post-treatment to show that functional tuning does not compromise mechanical robustness.\n7. If nanophase reconfiguration is driven by competitive interactions among salts, polymer, solvent, and PEDOT:PSS, then other interaction‐modulation approaches (e.g., changing solvent polarity or adding co-solvents) should also work. Consider complementary experiments—such as varying solvent composition—to validate your proposed mechanism.\nMinor Comments\n8. The Introduction is overly long. Please streamline it by focusing on the key advances of this work; move detailed technical descriptions to the Results & Discussion.\n9. In the device demonstrations, long-term stability may be compromised by solvent evaporation and sensitivity to environmental ions. Please comment on operational lifetimes."}, "author_response": "Point-by-Point Response to Reviewers’ Comments\n(Black italic: Reviewer’s remarks; Blue: Our response)\nDear Reviewers,\nThank you for your valuable time and constructive comments to help further improve the\nmanuscript. We have adjusted certain statements, conducted additional characterizations, and\nadded further elaboration.\nHere is a brief list of the major changes:\n1. Providing more detailed descriptions of the fabrication process of organogels and related\ndevices to enhance reproducibility.\n2. Revising the abstract and introduction section to better highlight the novelty and\nsignificance of this work.\n3. Clarifying the concept of mechanical-electrical decoupling and compared our system with\npreviously reported results.\n4. Systematically examining the interaction among conducting polymers, PVA, Ca2+ and\nglycerol through additional characterization.\n5. Deepening the mechanistic understanding of nanophase reconfiguration through a series of\nadditional control experiments and characterizations.\n6. Investigating the environmental stability and mechanical robustness of organogel-based\ndevices under various conditions.\n7. Evaluating the biocompatibility of the developed organogels through both in vitro and in\nvivo tests.\n8. Extending the reversible nanophase regulation strategy to other material systems\ncomprising conductive components (such as Ag, polyaniline), insulative components (such\nas polyacrylamide), and alternative disperse media (such as polyglycerol).\n9. Revising the manuscript throughout to improve conciseness and coherence.\n10. Correcting the format errors of figures.\nComment 1\nZhong et al reported on \"Highly reconfigurable neuron-mimicking conductive networks\nthrough nanophase structure engineering\" This research introduces a novel strategy for\ndeveloping next-generation bionic electronics by leveraging specific ion-mediated reversible\nnanophase reconfiguration within conductive organogels. The manuscript presents significant\nprocess in dynamic material engineering. However, there are critical concerns regarding the\nbiomedical relevance and lack of physiological compatibility validation. To support their claims,\nadditional confirmation is needed, as outlined below. Hence, we opted for a minor revision of\nthese findings\nResponse:\nWe appreciate your encouraging comments. We have performed additional characterizations\nand provided further elaboration to address your concerns, including biocompatibility, cell\nmorphological analysis, in vivo compatibility, etc, as detailed point-by-point below.\nComment 2\nLack of biocompatibility evaluation: the organogels developed in this work are intended for\ndirect or semi-direct contact with biological tissue (e.g., skin-mounted digital wristbands for\nEMG recording). However, the manuscripts dose not present any biocompatibility assessment,\nsuch as cytocoxicity, hemocompatibility, or inflammation-related assays. Inclusion of in vitro\ncell viability studies is strongly recommended to confirm safety for on-skin or in vivo use. We\nrecommend referencing biocompatibility evaluation methods as demonstrated in “Lubricant-\ninfused Polymeric Interfaces: A stretchable and anti-fouling surface for implantable\nbiomaterials (Adv. Funct. Mater. 2024)”, which provided a clear protocol for cell viability and\ncell aspect ratio analysis for biomedical application. Adoption similar in vitro testing methods\nwould significantly support the claimed biomedical applicability of the CP-PVA organogels.\nResponse:\nThank you for your helpful suggestions. We have included a systematic biocompatibility\nassessment in the revised manuscript, following the methodology described in the previous\nliterature (Adv. Funct. Mater., 2024, 34, 2312740), encompassing both in vitro\ncytocompatibility tests and in vivo biocompatibility studies.\nFirst, the in vitro cytocompatibility of CP-PVA organogels was evaluated through\nLive/Dead staining analysis and cell morphological analysis. Fibroblast cells were cultured in\na two-chamber Transwell system with a CP-PVA organogel placed in the transwell insert\n(Figure R1a). According to the Live/dead staining analysis, the CP-PVA organogels exhibited\nno apparent cytotoxicity, comparable to the control group (medium only), as revealed by\npredominantly green fluorescence (live cells) and negligible red fluorescence (dead cells) in the\nCP-PVA organogel groups (Figure R1b). Moreover, the good cytocompatibility was further\nconfirmed by cell morphological analysis, where no significant difference in cell aspect ratio\nwas observed between the CP-PVA organogel (lower panel) and control groups (upper panel)\nafter 24 h and 48 h of culture (Figure R1c, d). This result suggested that the CP-PVA organogels\ndid not adversely affect cell spreading or morphology.\nCP-PVA organogels in female SD (Sprague-Dawley) mice (Figure R1e). The incisions healed\nsmoothly after implantation without obvious signs of exudation, erythema, or swelling. The\nsurrounding tissues maintained intact structures with no obvious evidence of inflammatory cell\ninfiltration, necrosis, or fibrotic responses through histological assessment with hematoxylin &\neosin (H&E) staining (Figure R1f). These observations collectively demonstrate the excellent\nbiocompatibility of the CP-PVA organogels.\nRevision:\n1. In detail, the good biocompatibility of CP-PVA organogels was a prerequisite for high-quality\nsignal acquisition, which was confirmed by both in vitro cytocompatibility tests and in vivo\nsubcutaneous implantation assessment (Supplementary Note 9, Supplementary Fig. 83)31, 32.\n(Line 4-7 Page 20 in the revised main manuscript)\n2. Supplementary information | In-vitro biocompatibility evaluation\nA two-chamber Transwell system (8 μm pore size; Corning) was used for biological\nevaluation, following the methodology described in the previous literature (Supplementary\nFig. 82a)1. CP-PVA organogels were placed on the Transwell inserts, and L929 fibroblast\ncells (0.5 × 105 counts mL−1) were cultured in 2 mL of Dulbecco’s modified Eagle medium\n(DMEM) supplemented with 10 vol% bovine calf serum and 1 vol% penicillin–streptomycin.\nCell viability was assessed using a Live/Dead assay kit (L3224, Invitrogen, USA) according\nto the manufacturer’s protocol, and visualized with an inverted fluorescence microscope\n(IX83, Olympus, Japan) at 10× magnification. For nuclear staining, L929 cell nuclei were\ncounterstained with DAPI (4′,6-diamidino-2-phenylindole) and imaged using a confocal\nlaser scanning microscope (TCS SP8, Wetzlar, Germany). The image analysis was performed\nusing the ImageJ/FIJI software package. The CP-PVA organogels used for the tests had a\nsolid content of ~50 wt% (relative to the total mass of organogels) and CP’s relative content\nof 22 wt% (relative to the total mass of CP and PVA). (Line 16-29 Page 10 in the revised\nSupplementary Information)\n3. Supplementary information | In-vivo biocompatibility evaluation.\nFemale SD mice (7 weeks old) were purchased from Jiangsu Qinglongshan Biotechnology\nCo., Ltd. (Nanjing, China) and quarantined under semi-specific pathogen-free (semi-SPF)\nconditions with a 12 h light/dark cycle. A ~15 mm longitudinal incision was made using\nsurgical scissors to expose the subcutaneous space after shaving the leg skin. Subcutaneous\npockets were then created with blunt forceps to accommodate a CP-PVA organogel with a\nsize of 1.0 cm × 0.5 cm. Following implantation, the incisions were closed with surgical\nsutures. The mice were monitored and maintained under controlled housing conditions for\none week. After one week, the mice were sacrificed, and tissue samples surrounding the\nimplanted CP-PVA organogels were carefully collected. The explanted tissues were fixed in\n4 vol% paraformaldehyde (PFA) solution overnight at room temperature and subsequently\nembedded in paraffin wax. Sections with a thickness of 3–5 μm were cut and mounted onto\nglass slides for histological staining. The inflammatory response was assessed by\nhematoxylin and eosin (H&E) staining, in which nuclei appear blue and cytoplasm pink. The\nCP-PVA organogels used for the tests had a solid content of ~50 wt% (relative to the total\n3\nmass of organogels) and CP’s relative content of 22 wt% (relative to the total m’ass of CP\nand PVA). (Line 30-39, Page 10, Line 1-6, Page 11 in the revised Supplementary\nInformation)\n4. Supplementary Note 9 | Biocompatibility of CP-PVA organogels.\nPEDOT:PSS, PVA, and glycerol are generally regarded as biocompatible and have been\nwidely reported in biomedical engineering applications such as tissue regeneration and\nbiosensing4-6. To further verify the biocompatibility of the CP-PVA organogels, both in vitro\nand in vivo evaluations were conducted. First, the in vitro cytocompatibility of CP-PVA\norganogels was evaluated through Live/Dead staining analysis and cell morphological\nanalysis. Fibroblast cells were cultured in a two-chamber Transwell system with a CP-PVA\norganogel placed in the transwell insert (Supplementary Fig. 83a). According to the\nLive/dead staining analysis, the CP-PVA organogels exhibited no apparent cytotoxicity,\ncomparable to the control group (medium only), as revealed by predominantly green\nfluorescence (live cells) and negligible red fluorescence (dead cells) in the CP-PVA\norganogel groups (Supplementary Fig. 83b). Moreover, the good cytocompatibility was\nfurther confirmed by cell morphological analysis, where no significant difference in cell\naspect ratio was observed between the CP-PVA organogel and control groups revealed after\n24 h and 48 h of culture (Supplementary Fig. 83c, d). This result suggested that the CP-PVA\norganogels did not adversely affect cell spreading or morphology.\nSecond, to assess the in vivo compatibility, we performed subcutaneous implantation of\nCP-PVA organogels in female SD (Sprague-Dawley) mice (Supplementary Fig. 83e). The\nincisions healed smoothly after implantation without obvious signs of exudation, erythema,\nor swelling. The surrounding tissues maintained intact structures with no obvious evidence\nof inflammatory cell infiltration, necrosis, or fibrotic responses through histological\nassessment with hematoxylin & eosin (H&E) staining (Supplementary Fig. 83f). These\nobservations collectively demonstrate the excellent biocompatibility of the CP-PVA\norganogels. (Line 1-23, Page 20 in the revised Supplementary Information)\nFigure R1 (Fig. 83 in the revised Supplementary Information). a Schematic illustration of\n4\nthe two-chamber Transwell system used for cytocompatibility assessment. b Live/Dead\nviability assays of bare group (medium only, upper panel) and CP-PVA organogel group (lower\npanel), suggesting the good in vitro cytocompatibility of CP-PVA organogel with mouse\nfibroblasts (NCTC clone 929). Scale bar, 50 μm. c, d Morphological assessment of cells\ncultured on the substrate in the two-chamber Transwell system. Scale bar, 20 μm. Cell nuclei\nare stained with DAPI (blue color) (Panel c), and the cell aspect ratios were compared between\nbare and CP-PVA organogel groups at 24 h and 48 h of culture (Panel d). The cell aspect ratio\nis defined as the ratio of the major to the minor cell axes. The data in panel d were presented in\nbox-and-whisker plots, where the central dots, lines, and box limits indicate the mean, the\nmedian, and the upper/lower quartiles, and the whiskers extend to 1.5× the interquartile range\nfrom the quartiles (sample size: 4). e, f In vivo biocompatibility evaluation of CP-PVA\norganogel through subcutaneous implantation in the leg of mice (e). The surrounding tissue at\nthe implantation site was frozen-sliced and stained with H&E after one week of implantation\n(f). Statistical significance was assessed using two-sided t-tests for comparisons between two\ngroups (panel d) with significance levels, denoted as p ≥ 0.05 (not significant, NS), p < 0.05(*),\np < 0.01(**), and p < 0.001(***). The CP-PVA organogels with a glycerol relative content of 4\nwt% (relative to the total mass of the precursor suspension) and a CP relative content of 22 wt%\n(relative to the total mass of CP and PVA) were used for the experiments.\nComment 3\nMechanical mismatch with skin tissue: The reported Young’s modulus of 2.8-13.5 MPa exceeds\nthat of soft biological tissue (typically 100-500 kPa for skin). For conformal applications, such\na mechanical mismatch may result in poor adhesion, skin irritation, or mechanical fatigue. If\nfor dermal interfacing, modulus adjustment strategies or design accommodations should be\nconsidered.\nResponse:\nThank you for your valuable comment. We fully agree that the relatively high Young’s modulus\nof the CP-PVA organogel reported in this work (> 1 MPa) may lead to mechanical mismatch\nwhen in contact with biological tissues (e.g., Young’s modulus of human epidermis: 0.42-0.85\nMPa).\nTo address this concern, we prepared CP-PVA organogel with reduced Young’s modulus\nby lowering the solid content of organogels (i.e., increasing the glycerol’s content). Specifically,\nthe Young’s modulus decreases monotonically with the reduction of solid contents, and reaches\n0.45 MPa at 9 wt%, which falls within the mechanical range of epidermal tissue (Figure R2a-\nc). The low-modulus CP-PVA organogel therefore exhibited excellent mechanical compliance\nand conformability to soft biological tissues and biomimetic structures such as fine fingerprint\ntextures and convoluted cerebral cortex models, but at a compromise in electrical conductivity\n(8.4 S cm−1) (Figure R2d-f). Additionally, we validated that CP-PVA organogels with low solid\ncontents retained the electrical reconfigurability with a high conductance on/off ratio of 7.3×103,\nindicating that the reduction in the solid contents did not compromise the dynamic functionality\nof the organogels (Figure R3).\nAdditionally, highly conductive organogels with a lower Young’s modulus are also\npromising to engineer by controlling the molecular weight or hydrolysis degree of PVA, or by\nintroducing other polymer systems that exhibit specific ion effect (e.g., polyacrylamide, Sci.\nwork—nanophase reconfiguration, the optimization of mechanical performance will be\nsystematically investigated in future studies.\nRevision:\n1. The p-CP-PVA organogels were free-standing and exhibited varied mechanical robustness\ndepending on the relative contents of each component (Supplementary Note 2 and\nSupplementary Figs 2-4). (Line 20-22, Page 6 in the revised main manuscript)\n2. The resultant organogels (CP-PVA) experienced significant improvement by 4-5 orders of\nmagnitude, reaching 4.6-112.5 S cm−1 depending on the CP’s contents in the organogels,\naccompanied by moderate improvement in mechanical performance and an increase in solid\ncontent of ~50 wt% (Figure 2a-d, Supplementary Figs 6 and 7). (Line 27-31, Page 6 in the\nrevised main manuscript)\n3. Supplementary Note 2 | Effect of CP’s content and solid content on the mechanical\nperformance of p–CP-PVA and CP-PVA organogels.\nTo tune the solid contents, precursor solutions with different glycerol concentrations (4-19\nwt%, relative to the total mass of suspension) were prepared, while fixing the CP’s content\nas 22 wt% (relative to the total mass of PVA and CP) (Supplementary Fig. 1b). The resulting\np-CP-PVA organogels therefore exhibited solid contents ranging from 7 wt% to 39 wt%.\nWith increasing the solid contents, Young’s modulus and fracture stress monotonically\nincreased from 0.11 to 9.3 MPa and from 0.18 to 11.1 MPa, accompanied by a significant\nincrease in fracture elongation from 164% to 853% (Supplementary Fig. 4a-c). After\nthermal annealing at 80 oC for 2 hours, corresponding conductive CP-PVA organogels with\nsolid contents of 9-50 wt% were obtained (Supplementary Fig. 1b). Their mechanical\nperformance followed a similar trend to that of the p-CP-PVA organogels. With the solid\ncontent increasing, the CP-PVA experienced a significant monotonic increase in Young’s\nmodulus (0.16 to 12.1 MPa) and fracture stress (0.22 to 16.7 MPa), with an increase in\nfracture elongation (185% to 679%) (Supplementary Fig. 4e-f). Particularly, a low Young’s\nmodulus of 0.43 MPa was achieved at solid contents of 13 wt%, which falls within the\nmechanical range of epidermal tissue. The low-modulus CP-PVA organogel, therefore,\nexhibited excellent mechanical compliance and conformability to soft biological tissues and\nbiomimetic structures, making it more suitable for bioelectronic applications. (Line 17-33,\nPage 13 in the revised Supplementary Information)\nMechanical and conductive properties of CP-PVA organogels with different solid contents (9-\n50 wt%, relative to the total mass of CP-PVA organogel): stress-strain rate of\n200% min−1 (a); fracture stress and fracture strain (b); Young’s modulus and toughness (c); and\nelectrical conductivity (d). The data in panel d was presented as box-and-whisker plot, where\nthe central dot and line indicate the mean and median, the box limits indicate the upper and\nlower quartiles and the whiskers extend to 1.5× the interquartile range from the quartiles\n(sample size: 4). e, f Photographs of CP-PVA organogels showing their excellent\nconformability to fingerprint textures and convoluted cerebral cortex models. The data in panels\nb and c were presented as mean values ± standard deviation (s.d.) (sample size: 4). Statistical\nsignificance was assessed using one-way analysis of variance (ANOVA) for comparisons\namong multiple groups (panel d), with significance levels, denoted as p ≥ 0.05 (not significant,\nNS), p < 0.05(*), p < 0.01(**), and p < 0.001(***). CP-PVA organogels with a CP relative\ncontent of 22 wt% (relative to the total mass of CP and PVA) were used for the experiments.\nThe solid contents of CP-PVA organogels were controlled by varying the glycerol’s relative\ncontents in the precursor solutions.\nregulation of CP-PVA organogels with different solid contents (relative to the total mass of\norganogels). a Electrical conductivity of CP-PVA organogels with different solid content at\ndifferent states in the first cycle. The transformation of organogels in State I was implemented\nthrough CaCl treatment (State II), dialysis in glycerol/water solution and drying (State III), and\n2\nthermal annealing (State I ). b Conductivity on/off ratio of CP-PVA organogels with different\n2\nsolid content in State I relative to those in State III. c Cyclic stability of CP-PVA organogels\nduring switching between high-conductance state (State I) and low-conductance state (State\nIII). The data are presented as mean values ± standard deviation (s.d.), with four different\nsamples examined in independent measurements. Statistical significance was assessed using\ntwo-sided t-tests for comparisons between two groups (panels a, c), and one-way analysis of\nvariance (ANOVA) for comparisons among multiple groups (panel b), with significance levels,\ndenoted as p ≥ 0.05 (not significant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***).\nComment 4\nRole of residual ions and skin exposure: the conductivity switching mechanism relies on Ca2+\nand other ions. However, the residual presence of these ions post-treatment (especially after\nCaCl exposer) is not clearly addressed. This raises concerns about ionic leaching, potential\n2\nlocal toxicity, and electrolyte imbalance when interfaced with biological systems.\nResponse:\nThank you for your valuable comments. In this work, CaCl salt treatment was employed to\n2\nerase the previously patterned conductive path in CP-PVA organogels. Afterward, dialysis in\nwater was performed to induce CP-PVA transformation from a thermodynamically favorable\nhigh-resistance state (State II) to a kinetically favorable high-resistance state (State III). During\nthis process, most Ca2+ ions were removed from the organogels, with residual Ca2+ content of\n~0.5% (relative to the carbon) according to X-ray photoelectron spectroscopy (XPS) (Figure\nthe extracellular calcium concentration in mammals is around 1 mM) (Tor Ø Grøndahl et al.,\nBrain Research, 1998, 796, 125-131).\nRevision:\n1. Furthermore, the resistance of State II was maintained or even further increased by dialyzing\nout Ca2+ ion with glycerol solution, followed by selective evaporation at an ambient\nenvironment, to produce State III (residual Ca2+ ion content: ~0.5% relative to the carbon,\nSupplementary Fig. 33 and Supplementary Table 5). (Line 20-24, Page 9 in the revised\nmain manuscript)\nFigure R4 (Fig. 33 in the revised Supplementary Information). XPS survey spectra of the\nCP-PVA organogel in different states. The residual Ca2+ ion was determined to be ~0.5%\n(relative to the carbon), which is expected to exert negligible biological toxicity, given that the\nextracellular calcium concentration in mammals is around 1 mM (Tor Ø Grøndahl et al., Brain\nResearch, 1998, 796, 125-131).\nTable R1 (Table 7 in the revised Supplementary Information). Elemental composition for\nCP-PVA organogel in different states.\nState I State II State III\nElements\n(%) (%) (%)\nC 72.4 66.9 73.3\nO 21.4 18.5 21.6\nS 6.2 5.0 4.7\nCa 0 9.6 0.4\nComment 5\nFor the EMG measurement section in Figure 6, it would be beneficial to include additional\nexperimental data, if available. Supplementary materials, such as a real-time measurement\nvideo, could further enhance the manuscript. Additionally, more detailed information regarding\nthe EMG measurement system is needed. Currently, only the electrodes are described, and there\nis limited discussion on how the system reliably captures such subtle biosignals. Considering\nthe challenges of maintaining a high SNR at micro- to millivolt scales, and given that the PCB\nappears to serve as a simple rigid connector, further technical details about the measurement\nequipment and sensors would strengthen the manuscript.\nWe sincerely appreciate your valuable suggestions. In the revised manuscript, we have included\ndetailed information on the EMG measurement system in the Experimental Section and added\nadditional impedance characterization as well as a real-time measurement video\n(Supplementary video 2). For EMG measurement, the digital wristband fabricated from CP-\nPVA organogel was connected to a biosignal acquisition board (Cyton board, OpenBCI, U.S.)\nvia a flexible printed circuit board (FPCB) as a connector. The connection to FPCB was\nachieved, following a conformal soldering method described in this work, in which the digital\nwristband was soldered to the FPCB using an aqueous CP/PVA solder through selective laser\nirradiation. The resulting electrical contact exhibited excellent reliability and robustness to\nmechanical deformation, as revealed by minimal change in the impedance of the wristband-\nFPCB system upon a tensile strain of 50% (Figure R5).\nRevision:\n1. Furthermore, compared to the previously reported bioelectrodes, the digital wristband\nshowed low electrical impedance and robust structural integrity while maintaining a stable\nelectrical connection when interfaced with a signal recorder via a PCB through a conformal\nsoldering method as described above (Fig. 6c, Supplementary Fig. 84, 85)33. Particularly, the\noverall impedance and phase angle of the digital wristband exhibited negligible changes\nunder 50% tensile stretching, demonstrating the excellent reliability of the system\n(Supplementary Fig. 86). (Line 7-13, Page 20 in the revised main manuscript)\n2. As an example, real-time monitoring of muscle activity was demonstrated by recording the\nsurface electromyography (sEMG) maps in space and time domains, highlighting potential\napplications in medical diagnosis or human-machine interaction (Fig. 6d, 6e, Supplementary\nFig. 88 and Supplementary Video 2). (Line 15-19, Page 20 in the revised main manuscript)\n2. A p-CP-PVA organogel (180 mm × 50 mm × 75 μm) was patterned into electrical traces by\na continuous laser (150 W m−2, wavelength: 532 nm, spot size: 0.3 mm, speed: 6 cm min−1)\nto fabricate a one-body digital wristband. The resulting digital wristband was connected to a\nbiosignal acquisition board (Cyton Board, OpenBCI, U.S.) via a flexible printed circuit board\n(FPCB) for EMG recording. The electrical connection between the wristband and the FPCB\nwas achieved using the conformal soldering method described above, where an aqueous\nCP/PVA solder was applied at the interface and selectively irradiated by laser (Fig. 6c). The\nacquired signals were wirelessly transmitted to a computer via Bluetooth and post-processed\nwith band-pass (0.5–100 Hz) and notch (50/60 Hz) filters. (Line 5-12, Page 27 in the revised\nmain manuscript)\nInformation). a Stable electrical connection of CP-PVA organogel to a FPCB. The CP-PVA\norganogel-based digital wristband could be spatially patterned through laser irradiation,\nallowing for multichannel board-to-board connections. b, c Impedance and phase angles of\ndigital wristband-FPCB system before and after 50% tensile stretching (Scale bar of inset, 0.5\nmm).\nComment 6\nFurther explanation of the erasing and rewriting process shown in Figure 6f would be helpful.\nThe current supplementary video appears to focus on the formation of a QR code, but does not\nclearly demonstrate the rewriting process. Including either direct experimental evidence or an\nillustrative depiction of the rewriting process would provide greater clarity for readers.\nResponse:\nThank you for your helpful suggestion. We have added detailed information on the erasing and\nrewriting process (as detailed below) in the Experimental Section of revised manuscript, and\nincluded two additional illustrative schematics along with representative photographs (Figures\nR6 and R7).\nRevision:\n1. Fabrication of in-situ rewritable electroluminescence devices\nOrganogel-based electroluminescence devices adopted a sandwich structure35, consisting of\na patterned organogel bottom electrode, an electroluminescent layer, an insulating layer, and\na Cu top electrode (Supplement Fig. 88). Patterned p-CP-PVA organogels (solid content: 40\nwt%, relative to the total mass of organogels, CP content: 22 wt% relative to the total mass\nof CP and PVA), serving as the bottom electrode, were prepared through laser irradiation as\n11\ndescribed above. The patterned p-CP-PVA organogels were then coated with a ZnS\nelectroluminescent layer through blade-coating uncured PDMS precursor containing ZnS\nparticles (mass ratio of PDMS to ZnS = 1:1.4) and solidifying in the ambient environment\n(25 ℃) for 4 hours. Next, barium powder was dispersed in uncured PDMS at a 1:1 mass ratio\nand applied atop the light-emitting layer to serve as the insulating layer, followed by curing\nin the ambient environment for 2 hours. Finally, conductive copper paste was applied to the\nsurface of the insulating layer to form the electrode layer. The EL devices were activated by\napplying an alternating current of 100 V and 3 kHz between the CP-PVA organogel and the\nconductive copper electrodes.\nTo reconfigure the electroluminescent pattern, a 15 wt% glycerol solution containing 2\nM CaCl2 solution was dropped onto the surface of the bottom electrodes in the EL devices\nand left static for 3 days, during which the previously patterned conductive traces were erased\n(Supplementary Figs. 90, 91). Then, CaCl2 was removed by repeated dialysis in a 15 wt%\nglycerol solution (four times), followed by partial drying in the ambient environment. The\nrecovered high-resistance organogel electrode was subsequently repatterned with new\nconductive traces via continuous laser direct writing, enabling the rewriting of the\nelectroluminescent pattern. (Line 14-33, Page 27 in the revised main manuscript)\nFigure R6 (Fig. 92 in the revised Supplementary Information). Schematic illustration\nshowing the fabrication process of the reconfigurable CP-PVA organogel-based EL device.\nshowing the reconfigurating process of the CP-PVA organogel-based EL device.\nComment 7\nThere are several instances throughout the manuscript where the arrangement of text and\nimages within the figures appears misaligned. For example, in Figure 1c,d, some text overlaps\nwith the images, and in Figure 3f, text seems to be misplaced, potentially leading to confusion\nabout the figure content. Overall, the quality and clarity of the figures do not fully meet the\nstandards expected for this journal, which makes it difficult to interpret the data. I recommend\na thorough revision of all figures to ensure proper alignment, clear labeling, and improved\noverall presentation.\nResponse:\nThank you for your suggestions. We have carefully checked all the figures and corrected the\nformatting mistakes, including Fig. 1; Fig. 2 e-g; Fig. 3e, f and h; Fig. 4c, d, j; Fig. 5b, c, h and\nj; Fig. 6a-c, h.\nComment 1\nThis paper introduces a novel strategy for designing reconfigurable bioelectronic materials by\nusing reversible nanophase regulation in dynamic, physically crosslinked conductive networks.\nThe organogels-based on conducting polymers (PEDOT:PSS), polyvinyl alcohol and\nglycerol—exhibit both significant electrical conductivity and excellent mechanical properties\nthanks to a nanophase separation which can be disturbed and recovered through an treatment\nwith kosmotropic cations Ca2+ (specific ion effect), dialysis and annealing. By this approach,\nfully characterized by numerous technics, the authors shows unique features such as micro-\npatternability, in situ solderability, recyclability, and global (annealing) or local (laser) control\nof the electronic conductivity. The proposed organogels show much better performances and\nstability that the corresponding hydrogels. This approach aims at mimicking the adaptability of\nbiological tissues, offering a promising route toward advanced bionic electronics. By this\noriginal approach, the authors demonstrate that their system overcomes the classical trade-off\nbetween electrical conductivity and dynamic mechanical behavior, thanks to the ion-induced\nmodulation of nanophase structure. They also show compatibility with rigid electronics (e.g.,\nflexible PCB), which is a major challenge in gel-based bioelectronics. The authors push the\neffort to the generalization of their approach with first results on other materials (e.g., Ag,\npolyaniline). To summarize my opinion, the paper is truly excellent and impressive, both from\nthe amount and the quality of the results. The significance of the achievements is high and all\nconclusions are strongly supported by numerous and relevant characterizations but also by\nseveral very convincing demonstrations. I am sure that this paper will be of great interest for\nthe community and I recommend its publication providing few minor revisions.\nResponse:\nWe sincerely appreciate your positive comments. We have added additional experiments and\ncharacterizations following your suggestions, as detailed below.\nComment 2\nCould the authors elaborate on the choice of the PEDOT:PSS grade? It is simply stated\n“Poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS, solid content: ~1.1\nwt%) was ordered from Heraeus Epurio Ltd” in the Materials section. Knowing that numerous\ngrades, with various molecular weight or various ratio between PEDOT and PSS are available,\ndoes any grade would be compatible with the proposed? Is the chosen grade the classical\n“PH1000” commonly used by the community?\nResponse:\nThank you for your helpful comment. In the main experiments, we used the PH 1000\nPEDOT:PSS from Heraeus Epurio Ltd. (solid content ~1.1-1.3 wt%, PEDOT:PSS mass ratio\n~1:2.5). This PEDOT:PSS grade was one of the most widely used formulations in the research\ncommunity, attributed to its high conductivity and excellent processability.\nTo verify the universality of our strategy across different commercial PEDOT:PSS systems,\nwe first conducted comparative experiments using another PEDOT:PSS grade, Orgacon™ ICP\n1050 (Sigma-Aldrich, solid content ~1.1 wt%, PEDOT:PSS ~1:2.5). The CP-PVA organogels\n14\nprepared from this formulation (CP -PVA) exhibited mechanical properties comparable to\nOrgacon\nthose derived from PH1000, with Young’s modulus of 2.5-18.5 MPa, fracture strains of 160%-\n970%, fracture strengths of 6.8-16.1 MPa, and toughness of 15.3-78.7 MJ·m−3 (Figure R8a-c),\ndepending on the CP contents. In terms of electrical properties, the CP -PVA organogels\nOrgacon\nalso showed good conductivities of 5.3-110.7 S·cm−1 (Figure R8d). Moreover, the reversible\nconductivity modulation behavior of the CP -PVA organogels were also observed, closely\nOrgacon\nmirroring that of the PH1000-based system: the organogels maintained high on/off ratios of\n2.5×103 to 6.1×103 (conductivity ratio between State I to State III) at relatively low CP contents,\nwhile the on/off ratio gradually decreased with increasing CP content (Figure R8e and f).\nAt last, to further elucidate the influence of the PEDOT-to-PSS ratio, we synthesized\nPEDOT:PSS samples with varied compositions (PEDOT:PSS ratios: 1:3, 1:4, and 1:5), and\nprepared a series of CP-PVA organogels (denoted as CP -PVA, CP -PVA,and CP -PVA,\n1:3 1:4 1:5\nrespectively). As the proportion of the insulating PSS content increased, the overall\nconductivity of the resultant organogels decreased as expected. Meanwhile, excessive PSS\nweakened the dynamic reconfigurability of the conductive network, as shown by the reduction\nin conductance on/off ratio with increasing PSS content (1.6×103, 106, 1.7 for organogels with\nPEDOT:PSS ratios of 1:3, 1:4, and 1:5, respectively) (Figure R9). This reduction in\nreconfigurability at high PSS contents probably arose from the relatively weak ion-specific\nresponsiveness of PSS compared with PVA, as well as the additional crosslinking effect of the\ndivalent kosmotropic cations (Ca2+) on PSS during electrical reconfiguration (discussed in\ndetail in the response below). As a whole, our proposed approach in this work showed good\ncompatibility with varied PEDOT:PSS systems, particularly with a relatively low content of\nPSS (PEDOT:PSS ratios: 1:2.5 to 1:4).\nFigure R8 (Fig. 54 in the revised Supplementary Information). a-c Digital photograph and\nmechanical properties of CP -PVA organogels with different relative content of CP\nOrgacon\n(relative to the total mass of CP and PVA): stress-strain curves recorded at a strain rate of\nOrgacon\n200% min−1 (a), summaries of fracture stress, fracture strain, toughness, and Young’s modulus\n(b, c). d Electrical conductivities of CP -PVA organogels with different relative content of\nOrgacon\nCP (relative to the total mass of CP and PVA). The data in panel d were presented in box-\nOrgacon\nand-whisker plots, where the central dots, lines, and box limits indicate the mean, the median,\n15\nand the upper/lower quartiles, and the whiskers extend to 1.5× the interquartile range from the\nquartiles (sample size = 4). e Conductance regulation of CP -PVA organogels with\nOrgacon\ndifferent relative contents of CP (relative to the total mass of CP and PVA). f Conductivity\nOrgacon\nratio of CP -PVA organogels in State I relative to those in State III. The data in panels b,\nOrgacon\nc, e and f were presented as mean values ± standard deviation (s.d.), with four samples tested\nin independent measurements. Statistical significance was assessed using two-sided t-tests for\ncomparisons between two groups (panels e), and one-way analysis of variance (ANOVA) for\ncomparisons among multiple groups (panels d and f), with significance levels, denoted as p ≥\n0.05 (not significant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***). The solid content of\nCP –PVA organogels used here were ~50 wt% (relative to the total mass of organogels).\nOrgacon\nFigure R9 (Fig. 55 in the revised Supplementary Information). Electrical reconfigurability\nof CP-PVA organogels derived from PEDOT:PSS with varied compositions (PEDOT:PSS\nratios: 1:3, 1:4, and 1:5) (denoted as CP -PVA, CP -PVAand CP -PVA, respectively). a-c\n1:3 1:4 1:5\nConductance regulation and cyclic stability of CP -PVA, CP -PVA and CP -PVA,\n1:3 1:4 1:5\norganogels during switching among different states. The transitions among different states were\nachieved following the same method described in the main manuscript. d-f Cyclic stability of\nCP-PVA organogels during repeated switching between State I and State III. g Conductivity\non/off ratio of CP-PVA organogels in State I relative to those in State III. All the data were\npresented as mean values ± standard deviation (s.d.), with four samples tested in independent\nmeasurements. Statistical significance was assessed using two-sided t-tests for comparisons\nbetween two groups (panels a-f), and one-way analysis of variance (ANOVA) for comparisons\n16\namong multiple groups (panel g), with significance levels, denoted as p ≥ 0.05 (not significant,\nNS), p < 0.05(*), p < 0.01(**), and p < 0.001(***). The solid content of CP-PVA organogels\nused here was ~50 wt% (relative to the total mass of organogels).\nRevision:\n1. At last, the proposed electrical reconfiguration strategy showed good generality across\ndifferent grades of PEDOT:PSS, alternative conductive fillers, and mechanical matrices\n(Supplementary Note 7, Supplementary Fig. 54-56). For example, the conductance\nreconfiguration was successfully achieved in organogels incorporating PEDOT:PSS with\nvarying PSS contents (PEDOT:PSS ratios ≤ 1:3) or employing other ion-sensitive\nmechanical components (e.g., polyacrylamide and PNIPAm). (Line 25-30, Page 12 in the\nrevised main manuscript)\n2. Synthesis of PEDOT:PSS with varying PSS contents\nPEDOT:PSS was synthesized via oxidative polymerization of 3,4-ethylenedioxythiophene\n(EDOT) in the presence of sodium polystyrene sulfonate (NaPSS, Mw: ~20 kDa). Briefly,\nEDOT monomer (50 μL, 47 mmol) was dispersed in 15 mL of NaPSS aqueous solution under\nvigorous stirring at room temperature, with the molar ratio of EDOT to the sulfonate units of\nNaPSS adjusted to be 1:3, 1:4, or 1:5. The mixture was stirred for 30 minutes to ensure\nuniform dispersion and effective interaction between EDOT and NaPSS. Subsequently,\nanhydrous ferric chloride (FeCl , 15.3 mg) and sodium persulfate (130 mg, 55 mmol) were\n3\nadded and the reaction were allowed to proceed under continuous stirring for 12 hours.\nDuring this period, the solution gradually turned dark blue, confirming the formation of\nPEDOT:PSS. Finally, the resulting dispersion were purified using cation- and anion-\nexchange resin to remove residual salts. (Line 22-31, Page 22 in the revised\nmain manuscript)\n3. Supplementary Note 7 | The generality of electrical reconfigurability\nTo verify the universality of our strategy across different commercial PEDOT:PSS systems,\nwe first conducted comparative experiments using another PEDOT:PSS grade, Orgacon™\nICP 1050 (Sigma-Aldrich, solid content ~1.1 wt%, PEDOT:PSS ~1:2.5). The CP-PVA\norganogels prepared from this formulation (CP -PVA) exhibited mechanical properties\nOrgacon\ncomparable to those derived from PH1000, with Young’s modulus of 2.5-18.5 MPa, fracture\nstrains of 160%-970%, fracture strengths of 6.8-16.1 MPa, and toughness of 15.3-78.7\nMJ·m−3 (Supplementary Fig. 54a-c), depending on the CP contents. In terms of electrical\nproperties, the CP -PVA organogels also showed good conductivities of 5.3-110.7\nOrgacon\nS·cm−1 (Supplementary Fig. 54d). Moreover, the reversible conductivity modulation\nbehavior of the CP -PVA organogels was also observed, closely mirroring that of the\nOrgacon\nPH1000-based system: the organogels maintained high on/off ratios of 2.5×103 to 6.1×103\n(conductivity ratio between State I to State III) at relatively low CP contents, while the on/off\nratio gradually decreased with increasing CP content (Supplementary Fig. 54e, f).\nNext, to further elucidate the influence of the PEDOT-to-PSS ratio, we synthesized\nPEDOT:PSS samples with varied compositions (PEDOT:PSS ratios: 1:3, 1:4, and 1:5), and\nprepared a series of CP-PVA organogels (denoted as CP -PVA, CP -PVA,and CP -PVA,\n1:3 1:4 1:5\nrespectively). As the proportion of the insulating PSS content increased, the overall\nconductivity of the resultant organogels decreased as expected. Meanwhile, excessive PSS\nwould weaken the dynamic reconfigurability of the conductive network, as shown by the\ndecreased conductance on/off ratio with increasing PSS content (1.6×103, 106, 1.7 for\norganogels with PEDOT:PSS ratios of 1:3, 1:4, and 1:5, respectively) (Supplementary Fig.\n55). This reduction in reconfigurability at high PSS contents probably arose from the\nrelatively weak ion-specific responsiveness of PSS compared with PVA, as well as the\nadditional crosslinking effect of the divalent kosmotropic cations (Ca2+) on PSS during\nelectrical reconfiguration (Supplementary Fig. 37). As a whole, our proposed approach in\nthis work showed good compatibility to varied PEDOT:PSS systems particularly with a\nrelative low content of PSS (PEDOT:PSS ratios: 1:2.5 to 1:4).\nAt last, we further extended this system to other conductive and structural systems. For\ninstance, PVA-based organogels prepared from other conductive fillers such as silver (Ag)\nand polyaniline (PANi) also exhibited comparable reconfigurable behavior. Moreover, the\nreconfiguration approach was successfully applied to organogels incorporating other salt-\nsensitive mechanical matrices, including polyacrylamide (PAM) and poly(N-\nisopropylacrylamide) (PNIPAm), further demonstrating the broad applicability of this\nmethodology (Supplementary Fig. 56). (Line 1-35, Page 18 in the revised Supplementary\nInformation)\nComment 3\nPlease carefully check if all the information on composition are provided for each steps. Indeed,\nthe various ratio investigated in the synthesis/characterization part of the manuscript makes it\nsometimes unclear which composition is chosen for subsequent experiments\nResponse:\nThank you for your reminder. We have added the detailed composition information in the\nrevised manuscript. Unless otherwise specified, CP-PVA organogels with a solid content of ~50\nwt% (relative to the total mass of organogels) and CP’s relative content of 22 wt% (relative to\nthe total mass of CP and PVA) were used, including electrical/mechanical tests, nanophase\nreconfiguration, and all demonstrations.\nRevision:\nUnless otherwise specified, CP-PVA organogels with a solid content of ~50 wt% (relative to\nthe total mass of organogels) and CP’s content of 22 wt% (relative to the total mass of CP and\nPVA) were used for the tests here. (Line 16-18, Page 6; Line 2-4, Page 11; Line 10-12, Page\n14; Line 18-20, Page 16; Line 18-19, Page 19; Line 1, Page 20 in the revised main\nmanuscript)\nComment 4\nIn the section “Mechanism on the nanophase structure reconfiguration”, the authors state that\n“In detail, the kosmotropic cations Ca2+ could bind with PVA chains to break the hydrogen\nbonds among them”. There is no mention of a possible interaction between cations and the\npolyanionic PSS.\nResponse:\nhydroxyl groups on PVA chains, Ca2+ could also interact with the PSS chains, which weakened\nthe reconfigurability, particularly at high PSS contents. To verify this, dynamic light scattering\n(DLS) measurements were conducted to examine the intermolecular interaction between PSS\nand Ca2+ ions. The addition of Ca2+ led to an increased hydrodynamic radius and positive shift\nof zeta potential of PSS in aqueous solution, revealing that the divalent cation can crosslink\nPSS chains (Figure R10).\nFurthermore, we investigated the impact of ionic crosslinking on the electrical\nreconfigurability of the CP-PVA organogels (Figure R9). As the PSS content increased, the\nconductivity on/off ratio decreased significantly. At low PSS contents (PEDOT:PSS ratio: 1:3),\nthe CP-PVA organogel exhibited excellent electrical reconfigurability, with a conductivity\nchange ratio of nearly three orders of magnitude between the high-conductance and the low-\nconductance states (Figure R9g). In contrast, the responsiveness of the organogels was\nmarkedly reduced at high PSS contents, resulting in a sharp reduction in the on/off ratio (e.g.,\none/off ratio: 1.7 for the PEDOT:PSS ratio of 1:5). These findings suggest that excessive PSS\nwill impair the effectiveness of Ca2+ as an erasing agent in the network. Therefore, CP-PVA\norganogels derived from PEDOT:PSS formulations with relatively low PSS content are\npreferred for achieving excellent electrical reconfigurability in the methodology proposed in\nthis work.\nFigure R10 (Fig. 35 in the revised Supplementary Information). a-f Zeta potential (a-c) and\nsize distribution (d-e) of PSS (a, d), PVA (b, e) and PSS-PVA mixture (c, f) in deionized water\nor CaCl aqueous solution (concentrations of PSS, PVA and CaCl were controlled to be 10 mg\n2 2\nml−1, 10 mg ml−1 and 20 mg ml−1).\nRevision:\n1. In detail, despite the Ca2+ could induce ionic crosslinking among partial PSS chains\n(Supplementary 35), these kosmotropic cations simultaneously interact with PVA chains,\nbreaking the hydrogen bonds among them, as confirmed by FT-IR, XRD, and SAXS spectra\n19\n(Fig. 3e and Supplementary Figs. 36, 37)29. (Line 14-17, Page 11 in the revised main manuscript)\n2. At last, the proposed electrical reconfiguration strategy showed good generality across\ndifferent grades of PEDOT:PSS, alternative conductive fillers, and mechanical matrices\n(Supplementary Note 7, Supplementary Fig. 54-56). (Line 25-27, Page 12 in the revised\nmain manuscript)\n3. Supplementary Note 7| The generality of electrical reconfigurability.\nTo verify the universality of our strategy across different commercial PEDOT:PSS systems,\nwe first conducted comparative experiments using another PEDOT:PSS grade, Orgacon™\nICP 1050 (Sigma-Aldrich, solid content ~1.1 wt%, PEDOT:PSS ~1:2.5). The CP-PVA\norganogels prepared from this formulation (CP -PVA) exhibited mechanical properties\nOrgacon\ncomparable to those derived from PH1000, with Young’s modulus of 2.5-18.5 MPa, fracture\nstrains of 160%-970%, fracture strengths of 6.8-16.1 MPa, and toughness of 15.3-78.7\nMJ·m−3 (Supplementary Fig. 54a-c), depending on the CP contents. In terms of electrical\nproperties, the CP -PVA organogels also showed good conductivities of 5.3-110.7\nOrgacon\nS·cm−1 (Supplementary Fig. 54d). Moreover, the reversible conductivity modulation\nbehavior of the CP -PVA organogels was also observed, closely mirroring that of the\nOrgacon\nPH1000-based system: the organogels maintained high on/off ratios of 2.5×103 to 6.1×103\n(conductivity ratio between State I to State III) at relatively low CP contents, while the on/off\nratio gradually decreased with increasing CP content (Supplementary Fig. 54e, f).\nNext, to further elucidate the influence of the PEDOT-to-PSS ratio, we synthesized\nPEDOT:PSS samples with varied compositions (PEDOT:PSS ratios: 1:3, 1:4, and 1:5), and\nprepared a series of CP-PVA organogels (denoted as CP -PVA, CP -PVA,and CP -PVA,\n1:3 1:4 1:5\nrespectively). As the proportion of the insulating PSS content increased, the overall\nconductivity of the resultant organogels decreased as expected. Meanwhile, excessive PSS\nwould weaken the dynamic reconfigurability of the conductive network, as shown by the\ndecreased conductance on/off ratio with increasing PSS content (1.6×103, 106, 1.7 for\norganogels with PEDOT:PSS ratios of 1:3, 1:4, and 1:5, respectively) (Supplementary Fig.\n55). This reduction in reconfigurability at high PSS contents probably arose from the\nrelatively weak ion-specific responsiveness of PSS compared with PVA, as well as the\nadditional crosslinking effect of the divalent kosmotropic cations (Ca2+) on PSS during\nelectrical reconfiguration (Supplementary Fig. 37). As a whole, our proposed approach in\nthis work showed good compatibility to varied PEDOT:PSS systems particularly with a\nrelative low content of PSS (PEDOT:PSS ratios: 1:2.5 to 1:4).\nAt last, we further extended this system to other conductive and structural systems. For\ninstance, PVA-based organogels prepared from other conductive fillers such as silver (Ag)\nand polyaniline (PANi) also exhibited comparable reconfigurable behavior. Moreover, the\nreconfiguration approach was successfully applied to organogels incorporating other salt-\nsensitive mechanical matrices, including polyacrylamide (PAM) and poly(N-\nisopropylacrylamide) (PNIPAm), further demonstrating the broad applicability of this\nmethodology (Supplementary Fig. 56). (Line 1-35, Page 18 in the revised Supplementary\nInformation)\nComment 5\nWhat happens to the content of PSS during the Ca2+ treatment/dialysis steps? In classical\nPEDOT:PSS systems, it is well-known that solvent annealing or washing can remove partly the\ninsulating PSS, leading to an enhancement of conductivity. What happens in this present case?\nCan the author provide evidence of the removal or not-removal of the component which is\ninitially present in a significant amount in the organogel?\nResponse:\nThank you for your suggestion. According to the X-ray photoelectron spectroscopy (XPS),\npartial removal of PSS occurred after CaCl treatment (in both State II and State III). In detail,\n2\nin the S2p fine-resolution spectra, the band at 166 eV corresponding to the PSS chain showed\na slight/moderate decrease in intensity relative to the PEDOT-related band at 161 eV, indicating\nthat approximately 15% of PSS was removed during CaCl treatment (Figure R11). It is\n2\nnoteworthy that the CP-PVA organogels remained high-resistance state after CaCl treatment\n2\n(State II) and maintained so after subsequent dialysis and partial drying (State III), further\nconfirming that the electrical conductivity of the organogel was primarily governed by their\nphase structures, as elaborated in this work, and was minimally affected by a moderate change\nof the composition.\n1. In addition, according to X-ray photoelectron spectroscopy, approximately 25% of PSS was\nremoved during CaCl treatment in the first cycle, further supporting that nanophase\n2\nstructural was the primary factors governing the electrical properties, rather than\ncompositional variations (Supplementary Fig. 39). (Line 27-30, Page 11 in the revised\nmain manuscript)\nFigure R11 (Fig. 39 in the revised Supplementary Information). a-c S2p XPS spectra of\nCP-PVA organogels in State I (a), State II (b), and State III (c) in the first switching cycle. In\ndetail, in the S2p fine-resolution spectra, the band at 166 eV corresponding to the PSS chain\nshowed a moderate decrease in intensity relative to the PEDOT-related band at 161 eV,\nindicating that approximately 15% of PSS was removed during CaCl treatment.\n2\nThis manuscript introduces a strategy termed nanophase structure engineering to develop\nhydrogel materials with tunable conductivity, enabling subsequent device fabrication via laser\nengraving. The overall concept is clearly presented, and the experimental work is thorough.\nHowever, several concerns regarding novelty and mechanistic interpretation remain. In its\ncurrent form, the work appears to be a combination of previously reported strategies without a\nsufficiently distinct innovation. The following comments outline key points that must be\naddressed to strengthen the manuscript’s contribution and justify its suitability for publication\nin Nature Communications.\nResponse:\nThank you for your valuable comments, which have helped us strengthen the quality of this\nmanuscript. We have addressed your concerns point-by-point below, including the\nbreakthroughs of this work, the detailed mechanism, the generality of the methodology, and the\ndevice stability.\nComment 1\nMany elements of the work closely resemble previously published studies: phase‐separation\nengineering (e.g., Nat. Mater. 22, 895–902 (2023)), solvent‐annealing to boost conductivity\n(e.g., Nat Commun 14, 2206 (2023)), the Hofmeister effect in conductive polymers (e.g., works\nfrom Xinmin He group), laser‐induced conductivity and adhesion in PEDOT hydrogels (e.g.,\nNat Electron 7, 475–486 (2024)), and conformal soldering techniques (Sci. Adv.10, eadp0730\n(2024)). The authors should clarify what is fundamentally new in their approach, explicitly\ncontrast it with these precedents.\nResponse:\nThank you for your valuable comments. The key novelty of this work lies in proposing a novel\nconcept and general methodology for reversible phase regulation to fabricate reconfigurable\nelectronics, thereby addressing a critical methodology gap related to spatial scales in the in-situ\nregulation of physical performance. In contrast, previous approaches to achieve electrical\nreconfigurability primarily relied on either macroscopic geometry engineering (Nat. Chem. Eng.\n2024, 1, 149; Sci. Robot. 2021, 6, eabd5483; Nature 2017, 541, 347) or molecular structure (\nor doping level) engineering (Nat. Mater. 2025, 24, 205-211; Science 2023, 380, 735-742; Nat.\nMater. 2020, 19, 969-973), which nevertheless struggled to integrate reconfigurability with\nexcellent electrical conductance and size scalability. The distinct academic idea and approach\nfurther differentiate this work from studies on the mechanical performance design of pure PVA\nhydrogel (Adv. Mater. 2021, 33, 2007829) as well as previously reported conductive-hydrogel\nrelated works which focused on developing specialized formulations for high\nelectrical/mechanical-performance (Nat. Mater. 2023, 22, 895; Nat. Commun. 2023, 14, 2206),\nadditive or subtractive manufacturing techniques (Nat. Mater. 2023, 22, 895; Nat. Electron.\n2024, 7, 475), or soldering methods (Sci. Adv. 2024, 10, eadp0730).\nBelow, we provided a detailed explanation of the key breakthroughs of this work and its\n22\npotential unique application scenarios:\nBreakthrough 1#: A New Methodology for Constructing in-situ Reconfigurable\nElectronics\nAs mentioned above, previous reported methodologies for constructing reconfigurable\nelectronic materials often inevitably led to compromised electrical performance (electrical\nconductance) and size scalability. This limitation stems from an intrinsic conflict between the\ndynamic properties and efficient charge transportation of electrically active materials: the\nformer usually necessitates the adaptive and weakly interacting building blocks, while the latter\nrequires highly conjugated or crystalline molecular structures with intimate electrical contacts\n(Nat. Commun. 2024, 15, 916; Nat. Photon. 2021, 15, 622).\nIn this work, by leveraging the high response of the nano-scaled phase structure of non-\ncovalently crosslinked networks to specific ions (i.e., ion-specific effect), we developed a next-\ngeneration reconfigurable conductive network. This network successfully integrated multiple,\ntraditionally contradictory properties—combining good electrical/mechanical performance\nwith excellent reconfigurability features such as micro-patternability and erasability of\nconductive pathways, in-situ wet solderability with good spatial resolution, and closed-loop\nrecyclability. In addition, we also proved the generality of this methodology by extending it to\nother material systems, including Ag–PVA, polyaniline (PANi)–PVAorganogels (Figure R12).\nBreakthrough 2#: Fundamental Understanding of the Thermodynamics and Kinetics of\nthe Phase Evolution Process of Non-Covalent Conductive Networks\nIn the previous study, the nanophase separation structure has been widely considered as a key\nfactor in preparing soft conductive elastomers/plastics that could decouple electrical and\nmechanical performances (Nat. Mater. 2023, 22, 895; Nature 2023, 614, 456; Nat Commun.\n2024, 15, 3071). However, as restrained in the understanding of the evolution process of phase\nstructure, lengthy trial-and-error experiments were usually required to obtain an optimum\ndesign with several parameters, including material type, molecular structure, surface\nmodification, and preparation procedures. In this work, we demonstrated that the specific ion effect\ncould be harnessed to delicately tune the intermolecular interaction for rational control over the\nnanophase structure and overall performance of the composite system. Building on this, we\nsystematically studied the thermodynamics and kinetics of phase structure evolution, which are\nshown to be governed by the delicate balance of inter- and intra-molecular non-covalent\ninteractions in the polymers. Importantly, because conventional time-temperature superposition\napproaches in polymer science may fail in the involatile functional hydrogel systems, our results show\nthat the specific ion effect provides an effective alternative toolbox for investigating their structure-\nperformance relationships through in situ regulating molecular interactions, without altering the material\ncomposition.\nImpact and Application Scenarios: Inspiring the Design of Reconfigurable Next-\nGeneration Devices\nThe proposed academic ideas with the methodology are expected to inspire the design of\nreconfigurable electronics with potential applications across diverse fields such as\nbioelectronics and smart electronics. Below, we highlight three promising application scenarios:\n1. Implantable devices with active softening ability\ndevices: the trade-off between high mechanical softness and processability during the\nimplantation process. Previously reported softening methods commonly rely on a passive\nprocess such as hydration (Nature 2023, 624, 295-302). By coupling the specific ion effect and\ncapacitive adsorption, implantable devices with active softening ability are expected to be\ndeveloped through capacitive adsorption of ions in body fluid under a small applied voltage.\n2. Next-generation anisotropic conductive film for neural interface\nBy laser micro-patterning, gel-based micropatterned conductive substrates can be developed\nwhile maintaining material components and structural integrity. They could serve as a\nreconfigurable platform to tune the growth and regeneration of neural tissue on both the spatial\nand temporal dimensions, enabling precise manipulation of neural circuits.\n3. Reconfigurable antenna for multichannel emergency communication\nNanophase structure control is expected to enable the design of reconfigurable conductive\nelastomers for re-writable and adaptive antennas. These antennas are expected to exhibit\nalterable electromagnetic characteristics (radiation frequency, polarization mode, and radiation\npattern) over a significantly wider range than previously reported metasurface antennas based\non doping-degree regulation of conducting polymers (Nat. Mater. 2025, 24, 205-211), allowing\nbroad and precise regulation of signal transmission and reception modes.\nRevision:\nWe have revised the Abstract and Introduction Sections in the revised manuscript to highlight\nthe novelty of this work.\n1. Benefiting from the dynamic response of noncovalent interaction to specific ions, the\ndeveloped system can successfully integrate multiple traditionally contradictory properties–\ncombining outstanding electrical/mechanical performance with excellent reconfigurability\nsuch as re-writability of conductive pathways, in-situ wet solderability with good spatial\nresolution, and closed-loop recyclability. (Line 20-25, Page 1 in the revised main\nmanuscript)\n2. By leveraging specific ion effect, the conductive network could be finely engineered,\neither locally or globally, to transition among different thermodynamic states with different\nnanophase structures, driven by the delicate balance of inter- and intra-molecular non-\ncovalent interactions of polymers (Fig. 1b). The unique capability enabled controlled spatial\nmodulation of electrical conductivity within a single system over a remarkable range of 4-5\norders of magnitude, without compromising structural integrity and mechanical robustness\n(Fig. 1c-e). (Line 31-35, Page 3, Line 1-2, Page 4 in the revised main manuscript)\n3. In the in-situ wet soldering, the Rec-CN could be directly joined to diverse substrates via\nlaser process or thermal treatment, while preserving its multichannel electrical connections\nand 3-dimensional (3D) geometric integrity, standing in contrast to previously reported\nhydrogel soldering methods which typically required intricate manual operation or were\nincompatible with 3D gels (Fig. 1f, g)23. (Line 4-8, Page 4 in the revised main manuscript)\n4. As a whole, we propose a reversible nanophase regulation strategy to address a critical\nmethodology gap in bridging the spatial scales for the in-situ regulation of electrical\nperformance in reconfigurable electronics. As a result, this approach successfully integrates\ngood electrical and mechanical performance with outstanding reconfigurability features,\nsuch as micro-patternability and re-writability of conductive pathways, in-situ wet\nsolderability with good spatial resolution, and closed-loop recyclability. (Line 14-19, Page\n4 in the revised main manuscript)\nFigure R12 (Fig. 56 in the revised Supplementary Information). a-d Conductance\nregulation and cyclic stability of Ag-PVA (a), PANi-PVA (b), CP-PAM (c),and CP-PNIPAm\n(d) organogels during switching among different states. The transitions among different states\nwere achieved following the same method described in the main manuscript. e-h Cyclic\nstability of Ag-PVA (e), PANi-PVA (f), CP-PAM (g) and CP-PNIPAm (h) organogels during\nrepeated switching between State I and State III. i Conductivity ratio of different organogels in\nState I relative to those in State III. All the data were presented as mean values ± standard\ndeviation (s.d.), with four samples tested in independent measurements. Statistical significance\nwas assessed using two-sided t-tests for comparisons between two groups (panels a-h), and\none-way analysis of variance (ANOVA) for comparisons among multiple groups (panel i), with\nsignificance levels, denoted as p ≥ 0.05 (not significant, NS), p < 0.05(*), p < 0.01(**), and p\n< 0.001(***).\nComment 2\nIn the synthesis of pristine CP-PVA organogels, drying the mixture at ambient conditions for\n24 h does not guarantee complete water removal because glycerol binds water via hydrogen\nbonding. Residual “bound” water may remain, and its amount will vary with the glycerol: water\nratio, significantly affecting the hydrogel’s final properties\nResponse:\nWe sincerely thank you for your valuable comments. We fully agree that “bound water” may\nremain in the organogels even after drying at room temperature for 24 h. Experimentally, to\nquantify the solvent composition, the glycerol in organogels was extracted by dialysis in a\n25\ndefined amount of water and quantified through high-performance liquid chromatography\n(HPLC) analysis, while the water contents were calculated from the solid and glycerol contents.\nTo clarify the influence of drying conditions, organogels were prepared under different drying\nhumidity at 25 oC (relative humidity: 20%, 50%, and 70%). The water content in the pristine\nCP-PVA organogels before thermal annealing (p-CP-PVA) increased from 5 wt% to 39 wt%\n(relative to the total mass of the organogels) with rising drying humidity (Table R2). The\nelevated water content led to a slight reduction in Young’s modulus and toughness of the p-CP-\nPVA organogels (Young’s modulus: 5.3 MPa to 4.0 MPa, fractural strength: 8.6 MPa to 6.1\nMPa, toughness: 47.1 to 37.5 MJ m−3, strain at break:809% to 763% for 20%, 50%, and 70%\nRH) (Figure R13).\nSubsequently, conductive CP-PVA organogels were prepared through thermally annealing\nat 80 °C under the corresponding humidity conditions. All samples exhibited comparable water\ncontents of ~4%, indicating that most of the water was removed during thermal annealing and\nthe process was largely insensitive to environmental humidity (Table R2). As a result, these\norganogels showed similar mechanical and electrical properties, with tensile strength of 15.6–\n16.3 MPa, modulus of 24.4-28.2 MPa, and conductivity of 23.3-29.3 S·cm−1 (Figure R14).\nFinally, considering that the drying step was also involved in the conductivity\nreconfiguration experiments, electrical reconfiguration was also performed under drying\nconditions with different relative humidities (20%, 50%, and 70% RH). The water content of\nCP-PVA organogel in State II and State III increased with rising environmental humidity (\nthe water content in State II: 8% to 38%, the water content in State III: 7% to 40% for 20%,\n50%, and 70% RH) (Table R2). Despite the fluctuation in water content, all samples remained highly\nresistant, consistent with the trend observed in the ambient environment (50% RH), indicating\nthat environmental humidity during the environmental humidity exerted a minimal effect on\nthe reconfigurability of the organogels (Figure R15).\nRevision:\n1. During this drying process, most water was selectively evaporated, leaving behind pristine\nCP-PVA organogels (p-CP-PVA) with solid contents of ~40 wt% and residual water contents\nof 22 wt% (relative to the total mass of organogels). The influence of environmental humidity\nduring drying is discussed in Supplementary Note 1 and summarized in Supplementary Table\n1. (Line 6-10, Page 5 in the revised main manuscript)\n2. Notably, the thermal annealing was largely insensitive to environmental humidity, as revealed\nby the comparable low residual water contents (~4%) in organogels treated under different\nrelative humidity levels (20-70%) (Supplementary Note 1, Supplementary Fig. 8 and\nSupplementary Table 1). (Line 31-34, Page 6 in the revised main manuscript)\n3. In addition, the conductance on/off ratios of CP-PVA organogels remained stable across a\nwide range of environmental humidity level, demonstrating the high reliability and\nreproducibility of their electrical reconfigurability (Supplementary Fig. 57). (Line 30-33,\nPage 12 in the revised main manuscript)\n4. Supplementary Note 1 | Effect of relative humidities in drying process on the electrical,\nmechanical performances, and reconfigurability of organogels.\nConsidering that drying at ambient conditions does not guarantee complete water removal in\nthe preparation of CP-PVA organogels and the residual “bound” water may impact their\nelectrical and mechanical properties, we performed controlled drying under different relative\nhumidity (RH) levels (20%, 50%, and 70% RH).\nExperimentally, to quantify the solvent composition of organogels, the glycerol in\norganogels was extracted by dialysis in a defined amount of water and quantified through\nhigh-performance liquid chromatography (HPLC) analysis, while the water contents were\ncalculated from the solid content and the glycerol content. With increasing drying humidity,\nthe water content in the pristine CP-PVA organogels before thermal annealing (p-CP-PVA)\nincreased from 5 wt% to 39 wt% (relative to the total mass of the organogels) (Supplementary\nTable 1). The elevated water content led to a moderate reduction in Young’s modulus and\ntoughness of the p-CP-PVA organogels (Young’s modulus: 5.3 MPa to 4.1 MPa, fractural\nstrength: 8.6 MPa to 6.1 MPa, toughness: 47.1 to 37.5 MJ m−3, strain at break: 809% to 763%\nfor 20%, 50%, and 70% RH) (Supplementary Fig. 2).\nSubsequently, these samples were thermally annealed at 80 °C under the corresponding\nhumidity conditions to obtain conductive CP-PVA organogels. All samples exhibited\ncomparable water contents of ~4%, indicating that most of the water was removed during\nthermal annealing and the process was largely insensitive to environmental humidity\n(Supplementary Table 1). As a result, these organogels showed similar mechanical and\nelectrical properties, with tensile strength of 15.6-16.3 MPa, modulus of 24.4-28.2 MPa, and\nconductivity of 23.3-29.3 S·cm−1 (Supplementary Fig. 8).\nFinally, considering that the drying step was also involved in the conductivity\nreconfiguration experiments, highly resistive CP-PVA organogels (CP-PVA organogel in\nState II and State III) were also prepared under drying conditions with different relative\nhumidities (20%, 50%, and 70% RH). Consistent with the trend observed in p-CP-PVA\norganogels as described above, the water content of CP-PVA organogel in State II and State\nIII increased with rising environmental humidity (the water content in State II: 8% to 38%,\nthe water content in State III: 7% to 40% for 20%, 50%, and 70% RH) (Supplementary Table\n1). Despite the fluctuation in water content, all samples maintained high resistance,\nindicating that environmental humidity during the drying process had a minimal effect on\nthe reconfigurability of the organogels (Supplementary Fig. 57). (Line 1-33, Page 12 in\nthe revised Supplementary Information)\nTable R2 (Table 1 in the revised Supplementary Information). Glycerol and water contents\nof p-CP-PVA and CP-PVA organogels prepared in different environmental humidity.\nRelative contenta CP-PVAc\nRH p-CP-PVAb\n(wt%) State I State II State III State I\n2\nglycerol 49 43 47 44 41\n~20%\nwater 5 3 8 7 2\nglycerol 38 45 37 37 42\n~50%\nwater 22 4 19 16 5\nglycerol 34 48 35 37 47\n~70%\nwater 39 5 38 40 4\n27\na Relative contents of glycerol and water in the organogels (relative to the total mass of\norganogels);\nb p-CP-PVA organogels were prepared by drying precursor suspension under different RH levels\nof 20%, 50%, and 70%) (Supplementary Note 1);\nc CP-PVA organogels were prepared by thermal annealing corresponding p-CP-PVA organogels\nunder different RH levels of 20%, 50%, and 70% (Supplementary Note 1), and their\ntransitions among differs state were performed following the treatment protocol described in\nthe main manuscript.\nFigure R13 (Fig. 2 in the revised Supplementary Information). a-c Mechanical properties\nof p-CP-PVA organogels prepared under drying conditions with different relative humidity\n(RH) levels (20%, 50%, and 70% RH): stress-strain curves recorded at a strain rate of 200%\nmin−1 (a), summaries of fracture stress, fracture strain, toughness, and Young’s modulus (b, c).\nThe data in panels b and c were presented as mean values ± standard deviation (s.d.), with four\nsamples tested in independent measurements.\nFigure R14 (Fig. 8 in the revised Supplementary Information). To study the impact of\nenvironmental humidity during thermal annealing, p-CP-PVA organogels with a solid content\nof ~40 wt% (relative to the total mass of the CP-PVA organogel) and a CP relative content of\n28\n22 wt% (relative to the total mass of CP and PVA) were thermally annealed at 80 °C for 2 hours\nunder different relative humidity (RH) conditions (Supplementary Note 1). a-c Mechanical and\nelectrical properties of CP-PVA organogels thermal annealed under 20-70% RH levels: stress-\nstrain curves recorded at a strain rate of 200% min−1 (a), summaries of fracture stress (b),\nfracture strain (b), toughness (c), and Young’s modulus (c), electronic conductivity (d). Data\nin panel d are presented in box-and-whisker plots, where the central dots, lines, and box limits\nindicate the mean, the median, and the upper/lower quartiles, and the whiskers extend to 1.5×\nthe interquartile range from the quartiles (sample size = 4). Data in panels b and c were\npresented as mean values ± standard deviation (s.d.), with four samples tested in independent\nmeasurements (sample size = 5). Statistical significance was assessed using one-way analysis\nof variance (ANOVA) for comparisons among multiple groups (panel d), with significance\nlevels, denoted as p ≥ 0.05 (not significant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***).\nFigure R15 (Fig. 37 in the revised Supplementary Information). a-c Conductance regulation\nand cyclic stability of CP-PVA organogels during switching among different states. The\ntransitions among different states were achieved following the same method described in the\nmain manuscript. In addition, the experiments were conducted under controlled environments\nwith relative humidity levels of 20% (a), 50% (b), and 70% (c), respectively. d-f Cyclic stability\nof CP-PVA organogels during repeated switching between State I and State III. g Conductance\non/off ratio of CP-PVA organogels in State I under different relative humidity (RH) levels (20%,\n50%, and 70% RH). The data are presented in box-and-whisker plots, where the central dots,\n29\nlines, and box limits indicate the mean, the median, and the upper/lower quartiles, and the\nwhiskers extend to 1.5× the interquartile range from the quartiles (Sample size = 4). The data\nin panels a-f were presented as mean values ± standard deviation (s.d.), with four samples tested\nin independent measurements. Statistical significance was assessed using two-sided t-tests for\ncomparisons between two groups (panels a-f), and one-way analysis of variance (ANOVA) for\ncomparisons among multiple groups (panel g), with significance levels, denoted as p ≥ 0.05\n(not significant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***). The CP-PVA organogels\nwith a CP relative content of 22 wt% (relative to the total mass of CP and PVA) were used for\nthe experiments.\nComment 3\nThe claim of successfully decoupling conductivity and toughness is not fully supported by\nFigure 2a–d. The hydrogel reaches maximum toughness at 22 wt % CP (27.3 S cm⁻¹) but highest\nconductivity at 34 wt % CP (112.5 S cm⁻¹) with much lower toughness (<12 MJ m⁻³). Selecting\nthe best values for each property under different conditions is misleading. Instead, report\nconductivity and toughness measured on the same sample batch or clearly explain why different\ncompositions should be compared side by side.\nResponse:\nWe sincerely appreciate your valuable comments. Following your suggestions, we have\nrevised the related descriptions to avoid potential misunderstanding by readers.\nIn most previous studies on conductive gels, the incorporation of rigid conductive\npolymers (CPs) often restricted the chain mobility of the insulative polymer and generated\nstress concentration regions at the interface, thereby inevitably reducing elongation (Table R3).\nIn contrast, in our system, the CP-PVA organogels not only maintained the excellent electrical\nconductivity of the CP component but also retained the excellent mechanical properties of pure\nPVA organogels. Notably, at CP contents below 28 wt%, the CP-PVA organogels showed\nsimultaneous improvement in stretchability and fracture strength when compared with the pure\nPVA organogels (Figure R16). The outstanding performance could be attributed to the\nsynergistic effect of CP and glycerol, where the former provided additional strong crosslinking\nnetworks, while the latter, serving as a plasticizer, effectively preserved the flexibility and\nmobility of PVA molecular chains at the same time. To further highlight this breakthrough, we\ncompared the performance of CP-PVA organogels with different CP contents to that of\npreviously reported systems, revealing their superior comprehensive mechanical–electrical\nperformance (Figure R17).\nTherefore, unlike conventional conductive gels that typically suffer from a trade-off\nbetween mechanical flexibility and electrical conductivity, our system successfully integrates\nboth advantages. The CP-PVA organogels thus achieve mechanical–electrical decoupling,\nenabling simultaneous optimization of mechanical robustness and electrical functionality.\nRevision:\n1. More importantly, when compared with the pure PVA organogel, the thermally-annealed CP-\nPVA organogel exhibited unexpected improvement in mechanical performance, which is in\nsharp contrast to most previous reports where the incorporation of rigid conductive fillers\ntypically led to embrittlement of the composites (Supplementary Table 2). (Line 38-39, Page\n6, Line 1-3, Page 7 in the revised main manuscript)\n30\n2. As a result, the PVA-CP organogels exhibited superior comprehensive performance in terms\nof conductivity, stretchability, and toughness when compared with previously reported\nconducting polymer hydrogels (Figure 2e, f, Supplementary Fig. 10 and Supplementary\nTable 3). (Line 7-10, Page 7 in the revised main manuscript)\nTable R3 (Table 2 in the revised Supplementary Information). Comparison between the\nCP-PVA organogel and other conductive gels.\nConduct Elongation at break\nRelative Change\nComponent ivity Ref.\ncontenta pristineb compositec ratiod\n(S cm−1)\nAdv. Mater.\nHydrophilic\n0.0635 2.5 wt% 700 35 −95% Technol. 2018, 3,\npolyurethane/PEDOT\n1800137\nHydrophilic Nat. Mater. 2023,\n11 22 wt% 700 300 −57%\npolyurethane/PEDOT 22, 895-902\nWaterborne Nat. Commun.\nNRe 8 wt% 200 100 −50%\npolyurethane/PEDOT 2020, 11, 4683\nPoly(N- J. Mater. Chem. A\nisopropylacrylamide)/P NRe 0.11 wt% 2500 1500 −40% 2019,7, 8204-\nEDOT 8209\nMater. Chem.\nChitosan/PVA/PEDOT 0.001 1 wt% 650 500 −23% Phys. 2019, 237,\n121882\nTyramine-modified Nat. Commun.\n0.018 1 wt% 500 400 −20%\nPVA/PEDOT 2021, 2082, 12\nNat. Commun.\nPVA/Polypyrrole 80 25 wt% 55 36 −35%\n2023, 14, 759\nACS Appl. Nano\nPVA/Polypyrrole NRe 4 wt% 270 230 −15% Mater. 2024, 7,\n25322–25334\nCP-PVA organogel\n0-11.6 8 wt% 761 992 +30% This work\n(PVA)\na Relative contents of conductive filler in the hydrogels (relative to the total mass of hydrogels);\nb Fracture strain of the pristine hydrogel before the incorporation of conductive fillers;\nc Fracture strain of the hydrogel after the incorporation of conductive fillers;\nd Change ratio of fracture strain after the incorporation of conductive fillers.\ne NR: Not reported\nInformation). a Electrical conductivities of CP-PVA organogels with different relative content\nof CP (relative to the total mass of CP and PVA). The data in panel a are presented in box-\nand-whisker plots, where the central dots, lines, and box limits indicate the mean, the median,\nand the upper/lower quartiles, and the whiskers extend to 1.5× the interquartile range from the\nquartiles (Sample size = 4). b-d Mechanical properties of C-PVA organogels with different\nrelative content of CP (relative to the total mass of CP and PVA): stress-strain curves recorded\nat a strain rate of 200% min−1 (b), summaries of fracture stress, fracture strain, toughness,\nand Young’s modulus (c, d). The data in panels c, d were presented as mean values ± standard\ndeviation (s.d.), with four samples tested in independent measurements. Statistical significance\nwas assessed using two-sided t-tests for comparisons between two groups (panel a), with\nsignificance levels denoted as p ≥ 0.05 (not significant, NS), p < 0.05(*), p < 0.01(**), and p <\n0.001(***). The CP-PVA organogels with a solid content of ~50 wt% (relative to the total mass\nof the CP-PVA organogel) were used for the experiments.\nstrain, and conductivity of CP-PVA organogels with different contents of CP (22 wt%, 28 wt%,\n34 wt%, relative to the total mass of PVA and CP), previously reported conducting polymer\nhydrogels. Data points are obtained from references mentioned in Supplementary Fig. 10 and\nSupplementary Table 3.\nComment 4\nGiven the critical role of annealing, the Methods section needs far more detail: Was annealing\nperformed in a controlled‐humidity chamber (dry annealing) or in a solvent bath (wet\nannealing)? What temperature, duration, and atmosphere were used? Furthermore, both CP and\nglycerol contents change during annealing; please decouple the effects of compositional shifts\nfrom nanophase restructuring.\nResponse:\nThank you for your helpful suggestions. In the revised manuscript, we have added detailed\nexperimental information about thermal annealing in the Methods section. Unless otherwise\nspecified, thermal annealing was performed at 80 °C under ambient conditions with a relative\nhumidity of 40%-60% and environmental temperature of ~25 oC. To better elucidate the effects\nof CP and glycerol on the nanoscale phase reconstruction, we prepared a series of CP-PVA\norganogels with different CP and glycerol contents. Their electrical and nanophase\nreconfigurability were systematically investigated.\nEffect of CP content\nWith increasing CP content from 10 to 34 wt%, the conductivity of CP-PVA organogels in State\nI gradually increased, reaching up to 112.5 S·cm⁻¹ at high CP levels (Figure R16a). However,\nthe conductance on/off ratio (conductivity ratio of State I to State III) decreased accordingly\n(8.5×103 to 50) with an inflection point at a CP content of 28 wt% (Figure R18). This trend\nindicated a weakened ion-specific response and dynamic adaptability in CP-PVA organogels\nwith high CP content, which could be ascribed to the enhanced π–π stacking between PEDOT\nchains at high CP levels. SAXS and AFM analyses further support this interpretation. In detail,\nCP-PVA organogels with low CP content showed clearly regulable phase structure as revealed\nby noticeable SAXS peak shifts and distinct morphological changes in AFM images between\nState I and State II (Figure R19 and R20). In contrast, organogels with high CP content showed\nonly minor SAXS peak shifts and minimal variation in AFM phase morphology. Therefore,\nincreasing CP content could facilitate the electrical conductivity of CP-PVA organogels,\nat a threshold of 28 wt%, beyond which the reconfigurability of the conductive networks would be\nsignificantly compromised.\nEffect of glycerol content\nAs the solid content decreased from 50 wt% to 9 wt% (roughly corresponding to a gradual\nincrease in glycerol content, though the relation is not strictly linear due to the flocculation of\nsolvent composition for the different organogels), the conductivity of the organogel decreased\nmonotonically, suggesting the partial disruption of conductive pathways (Figure R21).\nNevertheless, the increase in glycerol content had a nearly negligible effect on electrical\nreconfigurability (Figure R22). Likewise, the reconfigurability of nanophase structure\nremained excellent across the examined glycerol range, as confirmed by the discernible SAXS\n33\npeak shifts and corresponding phase-structure variations in AFM (Figure R23, 24). This result\nsupported the generality of the electrical reconfigurations.\nRevision:\n1. To further validate this mechanism, three sets of control samples were prepared, including\nCP-PVA organogels with varying CP contents or solid contents, CP-PVA hydrogels or\norganogels derived from other organic solvents, and chemically crosslinkable CP-PVAMA\norganogels (PVAMA: methacrylate modified PVA) (Supplementary Figs. 40-53). The\ndetailed discussion is provided in Supplementary Note 6. In brief, the control experiments\nfurther proved that the electrical reconfigurability originated from the dynamic response of\npolymers. Specially, organogels remained high on/off ratios of 103-104 across a wide range\nof CP content, but the ratio declined markedly at high loadings beyond a critical threshold of\n34 wt% (Fig. 3h) (Line 7-15, Page 12 in the revised main manuscript)\n2. Supplementary Note 6 | Control experiments of electrical reconfiguration.\nTo further confirm the mechanism of electrical reconfiguration, three sets of control samples\nwere prepared, including CP-PVA organogels with varying CP contents or solid contents,\nCP-PVA hydrogels or organogels from other solvents, and chemically crosslinkable CP-\nPVA organogels (PVA : methacrylate modified PVA) (Supplementary Fig. 40-50).\nMA MA\nIn detail, (i) for the PVA-CP organogels with varying CP contents or solid contents,\nincreasing the CP content or solid contents benefited the overall conductivity of the\norganogels but compromised the conductance on/off ratio (Supplementary Fig. 40 and 44).\nThis could be attributed to the lower chain dynamics due to the enhanced, as confirmed by\nthe SAXS and AFM analyses (Supplementary Fig. 41, 42, 45, and 46); (ii) For the glycerol-\nfree CP-PVA hydrogels or organogels from other solvents, the conductivity on-off ratio of\norganogels showed a strong correlation with the hydrogen-bond-related Hansen solubility\nparameter (δ ) of the solvent (Supplementary Table 6). Organogels prepared with high-δ\nh h\nsolvents, such as glycerol and diglycerol, exhibited pronounced conductivity modulation\n(9.5×103 and 7.3×103), whereas those derived from low-δ solvents (e.g., DMSO and DMF)\nh\ndisplayed much weaker switching behavior (9.0 and 10.4) (Fig. 3i, Supplementary Fig. 51-\n53). This trend aligned well with the reported plasticization capability sequence of\nPEDOT:PSS additives, where high-δ additives enhance film stretchability by disrupting\nh\ninterchain PSS interactions through hydrogen bonding (Supplement Table 6)2, 3; (iii) For the\nCP-PVA organogels, once the PVA were chemically crosslinked in previous, conductive\nMA MA\npercolation networks could no longer be formed even upon the application of thermal\nannealing. Instead, the CP-PVA organogels, if not crosslinked, could be regulated between\nMA\na high conductance state and a high resistance state by the specific ion effect, similar to its\nCP-PVA counterparts (Supplementary Fig. 49, 50). This phenomenon further confirmed the\nessential role of chain dynamics in the conductance tunability of the CP-PVA composite\nsystem. (Line 1-25, Page 17 in the revised Supplementary Information)\nof CP-PVA organogels with different contents of CP (relative to the total mass of CP and PVA)\nat different states in the first switching cycle. The CP-PVA organogels with solid content of 50\nwt% in State I were employed for the tests. The transformation of organogels in State I was\nimplemented through CaCl treatment (State II), dialysis in glycerol/water solution and drying\n2\n(State III), and thermal annealing (State I ). b Conductance on/off ratio of CP-PVA organogels\n2\nin State I relative to those in State III. c Cyclic stability of CP-PVA organogels during switching\nbetween high-conductance state (State I) and low-conductance state (State III). The data are\npresented as mean values ± standard deviation (s.d.), with four different samples examined in\nindependent measurements. Statistical significance was assessed using two-sided t-tests for\ncomparisons between two groups with significance levels (panels a, c), and one-way analysis\nof variance (ANOVA) for comparisons among multiple groups (panel b), denoted as p ≥ 0.05\n(not significant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***).\ndifferent contents of CP, including a low content of CP sample (22 wt%) and a high content of\nCP sample (34 wt%), were used for the experiments. The solid contents of CP-PVA organogels\nin State I were ~50 wt%. a, b AFM characterizations of CP-PVA organogels with different\ncontent of CP in different states: height image (upper panel) and phase image (bottom panel)\n(scale bar = 500 nm).\nFigure R20 (Fig. 42 in the revised Supplementary Information). a, b SAXS profiles of CP-\nPVA organogels with 22 wt% (a) and 34 wt% (b) relative content of CP in different states. CP-\nPVA organogels with ~50 wt% solid content (relative total mass of organogel) were used for\nthe experiments. When compared to that in State I, the scattering peak of CP-PVA organogels\n36\n(22 wt% relative content of CP) in State II weakened with a negative shift (corresponding to\nthe increase in average interphase distance). Such a transformation indicated that the CaCl\n2\ntreatment induced the partial disassociation of PVA crystalline domains. In comparison, the\nCP-PVA organogels (34 wt% relative content of CP) remained nearly intact toward CaCl\n2\ntreatment, revealing that the high dynamics of CP-PVA organogels mainly originated from\nPVA chains.\nFigure R21 (Fig.4 in the revised Supplementary Information). a-d Mechanical and\nconductive properties of CP-PVA organogels with different solid contents (9-50 wt%, relative\nto the total mass of CP-PVA organogel): stress-strain curves at a strain rate of 200% min−1 (a);\nfracture stress (b), Young’s modulus (c), and electrical conductivity (d). The data in panel a are\npresented in box-and-whisker plots, where the central dots, lines, and box limits indicate the\nmean, the median, and the upper/lower quartiles, and the whiskers extend to 1.5× the\ninterquartile range from the quartiles (sample size = 4). The data in panels c-d were presented\nas mean values ± standard deviation (s.d.) (sample size = 4). CP-PVA organogels with a CP\nrelative content of 22 wt% (relative to the total mass of CP and PVA) were used for the experiments.\nThe solid contents of CP-PVA organogels were controlled by varying the glycerol’s relative\ncontents in the precursor solutions.\nof CP-PVA organogels with different solid contents. a, b Electrical conductivity (a) of CP-PVA\norganogels in State I and State III in the first cycle and the corresponding conductance on/off\nratio (conductance ratio of State I to State III) (b). c Cyclic stability of CP-PVA organogels\nduring switching between high-conductance state (State I) and low-conductance state (State\nIII). CP-PVA organogels with 22 wt% relative content of CP were used for the experiments.\nThe data are presented as mean values ± standard deviation (s.d.), with four different samples\nexamined in independent measurements. Statistical significance was assessed using two-sided\nt-tests for comparisons between two groups with significance levels (panels a, c), and one-way\nanalysis of variance (ANOVA) for comparisons among multiple groups (panel b), denoted as p\n≥ 0.05 (not significant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***).\nimages of CP-PVA organogels with different solid content (50wt% and 69 wt%, relative to the\ntotal mass of organogel): height image (upper panel) and phase image (bottom panel) (Scale\nbar, 500 nm). The CP content of CP-PVA organogels used here was controlled to be 22 wt%.\nFigure R24 (Fig. 46 in the revised Supplementary Information). a, b SAXS profiles of CP-\nPVA organogels with different solid contents (50 wt% and 69 wt%, relative to the total mass of\norganogel). a, b SAXS profiles of CP-PVA organogels with different solid contents (50wt%\nand 69 wt%, relative to the total mass of organogel). The CP content of CP-PVA organogels\nused here was controlled to be 22 wt%. When compared to that in State I, the scattering peak\n39\nof CP-PVA organogels (50 wt% relative solid content) in State II weakened with a negative\nshift (corresponding to the increase in average interphase distance). Such a transformation\nindicated that the CaCl treatment induced the partial disassociation of PVA crystalline domains.\nCaCl treatment, revealing that higher glycerol content contributed to the enhanced molecular\n2\nchain dynamics in CP–PVA organogels.\nComment 5\nThe in-depth characterization focuses on CP-PVA interactions but largely overlooks the role of\nglycerol, which comprises a large fraction of the material and forms strong hydrogen bonds\nwith PVA. Please discuss how glycerol influences nanophase formation and mechanical\nbehavior. Additionally, since PEDOT:PSS contains both PEDOT and PSS, specify which\nmoiety interacts with PVA while discussing.\nResponse:\nWe sincerely thank you for the insightful comments. In the revised manuscript, we have\nclarified the role of glycerol in nanophase reconstruction and mechanical properties, as well as\ndiscussed the interaction of PEDOT:PSS and PVA. In the CP-PVA organogel system, glycerol\nformed abundant hydrogen bonds with PVA and CP, markedly affecting nanophase formation\nand macroscopic behavior. Regarding the interaction of PEDOT:PSS and PVA, the sulfonic\nacid group of PSS chains formed hydrogen bonds with the hydroxy groups of PVA.\nEffect of glycerol on phase structure and mechanical performance\nGlycerol exerted two principal effects on CP-PVA organogels. First, it served as a polar solvent,\nable to induce the conformational transition of PEDOT:PSS from a benzoid (coiled) to a quinoid\n(extended-coil) structure through screening effect, as previously reported (Nat. Biotechnol.\n2020, 38, 1031). This transformation was evidenced by the Raman shift of the C =C symmetric\nα β\nvibration from 1421 cm−1 to 1428 cm−1, which benefited the formation of conductance networks.\nSecondly, it acted as a plasticizer for both PVA and CP phases. The stretching peak of\nhydroxyl groups in PVA red-shifted from 3267 to 3259 cm−1, and XRD showed decreased\ncrystallinity (crystalline domain size reduced from 4.3 to 1.6 nm) after glycerol incorporation,\nindicating that glycerol disrupted PVA-PVA hydrogen bonds (Figure R25). Similarly, glycerol\ncould suppress the stacking of PEDOT:PSS chains through forming hydrogen bonds with PSS\nchains, according to a previous study (Macromolecules 2021, 54, 1234).\nThe plasticizing effect greatly suppressed dense aggregation and enhanced polymer\nmobility. With increasing glycerol content (i.e., decreasing solid contents), the organogels\ndisplayed significantly lower Young’s modulus and higher stretchability, indicating the\ndisruption of partial crosslinking sites (Figure R21 b-d). More importantly, the enhanced\ndynamics markedly facilitated nanophase reconfigurability. For instance, CP-PVA organogels\nwith low glycerol content showed weaker phase-structural changes upon CaCl treatment,\n2\nwhereas those with higher glycerol content displayed more distinct nanophase transitions\n(Figures R23, R24). This trend was consistent with their higher conductance on/off ratio\n(8.3×103) than that (1.4) of their hydrogel counterparts. Moreover, the essential role of\nplasticization in facilitating phase reconfigurability was further verified by control experiments\nusing alternative solvents, as detailed in our response to comment 7.\nchains, weakening their interchain interactions and thereby improving both mechanical\ncompliance and phase reconfigurability of the organogels.\nThe interaction of PEDOT:PSS and PVA\nThe interaction between the conducting polymer and PVA mainly originated from hydrogen\nbonding between PSS and PVA, as evidenced by dynamic light scattering (DLS), Fourier-\ntransform infrared spectroscopy (FT-IR) and mechanical testing.\nFirst, the zeta potential of PEDOT:PSS or PSS colloids in water before and after the addition\nof PVA was measured. Upon introducing PVA, the zeta potential of PEDOT:PSS increased from\n−49 mV to −39 mV, and that of PSS increased from −57 mV to −51 mV, indicating the\npronounced intermolecular interaction between PVA and PSS (Figure R26). In the FT-IR\nspectra, the sulfonic group in PSS and the hydroxy groups of PVA experienced obvious red\nshifts upon mixing, confirming the formation of a hydrogen bond between them (Hydroxy\ngroups in PVA: 3481 cm−1 to 3303 cm−1; sulfonic groups in PSS: 1193 cm−1, 1128 cm−1 and\n1039 cm−1 to 1184 cm−1, 1124 cm−1, and 1035 cm−1) (Figure R27).\nAt last, the interaction was further supported by the mechanical properties of PVA and\nPVA-PSS organogels. As the PSS content increased from 0 to 20 wt% (relative to the total mass\nof PVA and PSS), the tensile strength decreased from 7.0 to 2.1 MPa, and the Young’s modulus\ndropped from 5.4 to 1.2 MPa, indicating that PSS effectively disrupted the intermolecular\nhydrogen-bond network among PVA chains. As a whole, strong hydrogen bonding between\nPSS and PVA governs their mutual interaction in the CP-PVA system (Figure R28).\nRevision:\nOn the others, the PVA and PSS chains in CP could strongly interact with each other through\nionic hydrogen bonds, according to dynamic light scattering (DLS) spectra, Fourier-\ntransform infrared (FT-IR), XRD spectra and mechanical tests (Fig. 2j, Supplementary Figs.\n24-28, Supplementary Table 4). Furthermore, the glycerol, serving as an effective plasticizer\nthrough multiple hydrogen-bond interactions with both PVA and CP, could greatly suppress\ndense self-aggregation and thus enhance the polymer miscibility (Supplementary Fig. 29)24.\n(Line 34, Page 7, Line 1-6, Page 8 in the revised main manuscript)\nCP-PVA film without glycerol and CP-PVA organogel over the wavelength range of 700-4000\ncm−1, with scan numbers of 16 and a resolution of 4 cm−1. The dried CP-PVA film without\nglycerol were prepared following a procedure similar to that for the organogels, except that\nglycerol was not introduced. The redshift of hydroxyl-group-related peak at ~3260 cm−1\nindicated the glycerol formed hydrogen bonds with PVA. b-d XRD patterns (b), average\ncrystallite sizes (c) and solid contents (d) of CP-PVA organogels with different contents of\nglycerol. A series of CP-PVA organogels with varying glycerol contents were prepared from\nsuspension containing a CP’s relative content of 22 wt% (relative to the total mass of the PVA\nand CP) and varied contents of glycerol (0 wt%, 4 wt%, 7 wt%, 10 wt%, relative to the total\nmass of the precursor suspension) (denoted as CP-PVA , CP-PVA , and CP-PVA ,\n4% 7% 10%\nrespectively). With increasing the glycerol contents, the crystalline sizes of PVA in organogels\ndecreased significantly, revealing glycerol disrupted the ordered stacking of PVA chains. The\ndata in panel c are presented in box-and-whisker plots, where the central dots, lines, and box\nlimits indicate the mean, the median, and the upper/lower quartiles, and the whiskers extend to\n1.5× the interquartile range from the quartiles (Sample size = 4). The stretching peak of\nhydroxyl groups in PVA red-shifted from 3267 to 3259 cm−1, and XRD showed decreased\ncrystallinity (crystalline domain size reduced from 4.3 to 1.6 nm) after glycerol incorporation,\nindicating that glycerol disrupted PVA-PVA hydrogen bonds. Statistical significance was\nassessed using ANOVA for comparisons among multiple groups (panel c), with significance\nlevels denoted as p ≥ 0.05 (not significant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***).\nPEDOT:PSS, and PVA in water were controlled to be 10 mg·mL−1. a, b Zeta potential of PSS\n(a) and PEDOT:PSS (b) in the presence or absence of PVA. Upon introducing PVA, the zeta\npotential of PEDOT:PSS increased from −49 mV to −39 mV, and that of PSS increased from\n−57 mV to −51 mV, indicating the pronounced intermolecular interaction between PVA and\nPSS.\nFigure R27 (Fig. 26 in the revised Supplementary Information). FT-IR spectra of dried PVA,\nPSS, PVA-PSS, and CP-PVA (without glycerol). FT-IR spectra were recorded over the\nwavelength range of 600–4000 cm−1, with scan numbers of 16 and a resolution of 4 cm−1. The\nsulfonic group in PSS and the hydroxy groups of PVA experienced obvious red shifts upon\nmixing, confirming the formation of hydrogen bond between them (Hydroxy groups in PVA:\n3481 cm−1 to 3303 cm−1; sulfonic groups in PSS: 1193 cm−1, 1128 cm−1 and 1039 cm−1 to 1184\ncm−1, 1124 cm−1, and 1035 cm−1).\nand PVA-PSS organogel was achieved following a method similar to that for CP-PVA\norganogels as described in the main manuscript. The PVA and PVA-PSS organogels had a\ncomparable solid content of ~40 wt% (relative to total mass of organogel). a-c Mechanical\nproperties of PVA and PVA-PSS organogels with different relative content of PSS (relative to\nthe total mass of PSS and PVA): stress-strain curves recorded at a strain rate of 200% min−1 (a),\nsummaries of fracture stress, fracture strain, toughness, and Young’s modulus (b, c). As the\nPSS content increased from 0 to 20 wt% (relative to the total mass of PVA and PSS), the\ntensile strength decreased from 7.0 to 2.1 MPa, and the Young’s modulus dropped from 5.4 to\n1.2 MPa, indicating that PSS effectively disrupted the intermolecular hydrogen-bond network\namong PVA chains. The data in panels b and c are presented as mean values ± standard deviation (s.d.),\nwith four different samples examined in independent measurements.\nComment 6\nThe authors demonstrate tunable conductivity via Hofmeister salts but do not report the\ncorresponding mechanical properties. After ion‐specific treatment and re-annealing, are\ntoughness or elasticity preserved compared to the untreated hydrogel? Please provide\nmechanical data post-treatment to show that functional tuning does not compromise mechanical\nrobustness.\nResponse:\nWe sincerely thank you for the valuable comments. In the revised manuscript, we have included\nthe mechanical performance data of the CP-PVA organogels after CaCl treatment (State II),\n2\ndialysis (State III), and subsequent re-annealing (State I ). The organogels in State II and State\nMPa and toughness of ~58 MJ·m−3, compared with 16.7 MPa, 82.3 MJ cm−3 of organogels in\nState I (Figure R29). This reduction was mainly attributed to the partial disruption of the\nhydrogen bonds of PVA by the salt ions. The compromise in mechanical performance appeared\n44\nto be an inherent issue associated with the electrical reconfiguration mechanism, which relied\non altering the co-assembly behavior of PEDOT:PSS and PVA. Nevertheless, the mechanical\nperformance showed good recoverability after thermal re-annealing (State I ), consistent with\n2\nthe reversible reconfigurability of electrical conductivity.\nRevision:\nThis transition also reduced the Young’s modulus and toughness by 62% and 30%,\nrespectively, with a slight change in solid content (51% to 44%; Supplementary Fig. 32).\nFurthermore, the resistance of State II was maintained or even further increased by dialyzing\nout Ca2+ ion with glycerol solution, followed by selective evaporation at an ambient\nenvironment, to produce State III (residual Ca2+ ion content: ~0.5% relative to the carbon,\nSupplementary Fig. 33 and Supplementary Table 5). In this state, the conductivity decreased\nto 3.3×10−3 S cm−1, while the mechanical performance and solid content remained stable.\nMoreover, State III could be reverted to the original high-conductance state by thermal\nannealing at 80 °C for 2 hours (State I ), recovering the initial electrical and mechanical\n2\nperformance (Supplementary Figs. 31, 32). (Line 19-28, Page 9 in the revised main\nmanuscript)\nFigure R29 (Fig. 32 in the revised Supplementary Information). a-c Mechanical properties\nof CP-PVA organogel in different states: stress-strain curves recorded at a strain rate of 200%\nmin−1 (a), summaries of fracture stress, fracture strain, toughness, and Young’s modulus (b, c).\nThe transitions between different states were induced in an organogel with 50 wt% solid content\nand 22 wt% CP content, following the methods detailed in the main manuscript. The data in\npanels b and c are presented as mean values ± standard deviation (s.d.), with four different\nsamples examined in independent measurements.\nComment 7\nIf nanophase reconfiguration is driven by competitive interactions among salts, polymer,\nsolvent, and PEDOT:PSS, then other interaction‐modulation approaches (e.g., changing solvent\npolarity or adding co-solvents) should also work. Consider complementary experiments—such\nas varying solvent composition—to validate your proposed mechanism.\nResponse:\nWe sincerely appreciate the reviewer’s valuable comments. To verify the generality of the\nproposed strategy for the electrical reconfiguration, a series of CP-PVA organogels were\nprepared using different solvents, including dimethyl sulfoxide (DMSO), N, N-\ndimethylformamide (DMF), ethylene glycol (EG), and diglycerol (3,3'-oxybis(propane-1,2-\ndiol). Their reconfigurability of electrical conductivities was evaluated following the same\n45\ntreatment procedure, similar to (CaCl treatment and dialysis), as in this work. Taking the\n2\nconductance on/off ratio as a benchmark, the reconfigurability of organogels was found to\ncorrelate strongly with the hydrogen-bond-related Hanse solubility parameters (δ ) (Table R4).\nh\nOrganogels derived from solvents with high δ , such as glycerol and diglycerol, demonstrated\nh\npronounced on/off conductivity modulation (9.5×103 and 7.3×103), while those based on low-\nδ solvents (such as DMSO and DMF) exhibited poor switching behavior (9.0 and 10.4) (Figure\nh\nR30-33). Notably, this trend was nearly consistent with the reported plasticizing ability\nsequence of PEDOT:PSS additives, where higher-δ additives enhanced film stretchability by\nh\ndisrupting PSS interchain interaction via hydrogen bonds (Macromolecules 2021, 54, 1234)\n(Figure R33, Table R4). These results therefore further confirmed that the phase structure\noriginated from the competition between the miscibility and self-aggregation of the\nPEDOT:PSS and PVA chains, and could be reconstructed through engineering these two driving\nforces.\nFigure R30 (Fig. 52 in the revised Supplementary Information). CP-PVA-EG and CP-PVA-\nDiglycerol organogels were fabricated using EG and diglycerol as solvents, respectively.\nDetailed preparation procedures are provided in the main manuscript. The organogels with a\n46\nrelative CP content of 22 wt% (relative to the total mass of PVA and CP). a-f Electrical\nconductivity (a-c) and cyclic stability (d-f) of CP-PVA-EG organogels with different solid\ncontents (23 wt%, 34 wt%, and 50 wt%). g-l Electrical conductivity (g-i) and cyclic stability (j-\nl) of CP-PVA-Diglycerol organogels with different solid contents (23 wt%, 34 wt%, and 50\nwt%). The transformation of organogels in State I was implemented through CaCl treatment\n2\n(State II), dialysis in organic-solvent/water mixture solution and drying (State III), and thermal\nannealing (State I ), following the method described in the main manuscript. The data are\n2\npresented as mean values ± standard deviation (s.d.), with four different samples examined in\nindependent measurements. Statistical significance was assessed using two-sided t-tests for\ncomparisons between two groups with significance levels, denoted as p ≥ 0.05 (not significant,\nNS), p < 0.05(*), p < 0.01(**), and p < 0.001(***).\nFigure R31 (Fig. 53 in the revised Supporting Information). Conductance on/off ratio of\nCP-PVA-EG and CP-PVA-Diglycerol organogels.\nDMF organogels were fabricated using dimethyl sulfoxide (DMSO) and dimethylformamide\n(DMF) as solvents, respectively. Detailed preparation procedures are provided in the main\nmanuscript. The organogels with a relative CP content of 22 wt% (relative to total mass of PVA\nand CP). a-f Electrical conductivity of CP-PVA-DMSO (a-c), and CP-PVA-DMF (d-f)\norganogels with different solid contents (23 wt%, 34 wt%, 50 wt%) at different states in the\nfirst cycle. g Conductance on/off ratio of CP-PVA-DMSO, and CP-PVA-DMF organogels. The\ntransformation of organogels in State I was implemented through CaCl treatment (State II),\n2\ndialysis in organic-solvent/water mixture solution and drying (State III), and thermal annealing\n(State I ), following the method described in the main manuscript. The data in panels are\n2\npresented as mean values ± standard deviation (s.d.), with four samples examined in\nindependent measurements. Statistical significance (panels a-f) was assessed using two-sided\nt-tests for comparisons between two groups with significance levels, denoted as p ≥ 0.05 (not\nsignificant, NS), p < 0.05(*), p < 0.01(**), and p < 0.001(***).\nEG, diglycerol. b Variations of the conductance on/off ratio of CP-PVA organogel with the δ\nh\nvalue of the solvent.\nTable R4 (Table 8 in the Supplementary Information). Hansen solubility parameters of the\nsolvents and PEDOT.\nDielectric\nSolvents T a δ (MPa1/2)b δ (MPa1/2)c δ (MPa1/2)d Ref.\nm d p h\nconstant\nGlycerol 18 17.4 12.1 29.3 42.5 1\nEthylene\n-13 17.0 11.0 26.0 37 2\nGlycol\nDiglycerol 11 16.1 25.6 24.8 15.7 2\nDMSO 19 18.4 16.4 10.2 46.7 1\nEthanol -114 15.8 8.8 19.4 29.4 2\nDMF -31 17.4 13.7 11.3 38.3 2\nPEDOT NRe 21.2 7.4 8.1 NR 1\na Melting point (T );\nm\nb Dispersion force (δ );\nd\nc Permanent dipole-dipole force (δ );\np\nd Hydrogen bonding (δ );\nh\ne NR: Not reported.\nReference:\ncompounds of multiple hydroxyl groups for their application as transparent stretchable\nconductors. Macromolecules 54, 1234-1242 (2021).\nbiopolymer aerogels-dealing with the solvent. Gels 1, 291-313 (2015).\nRevision:\n1. Moreover, the conductance on/off ratio strongly correlated with the plasticization ability of\ndispersion media (solvent) in the organogels, specifically the hydrogen-bond-related Hansen\nsolubility parameter (δ ). Solvents with higher δ , which could offer more hydroxy groups\nh h\nfor interaction with PSS and PVA24, impart greater adaptability to the polymer network,\nthereby enhancing the electrical reconfigurability of corresponding organogels (Fig. 3i,\nSupplementary Figs. 51-53 and Supplementary Table 6). (Line 15-20, Page 12 in the revised\nmain manuscript)\n2. Supplementary Note 6 | Control experiments of electrical reconfiguration.\n(ii) For the glycerol-free CP-PVA hydrogels or organogels from other solvents, the\nconductivity on-off ratio of organogels showed a strong correlation with the hydrogen-bond-\nrelated Hansen solubility parameter (δ ) of the solvent (Supplementary Table 6). Organogels\nh\nprepared with high-δ solvents, such as glycerol and diglycerol, exhibited pronounced\nh\nconductivity modulation (9.5×103 and 7.3×103), whereas those derived from low-δ solvents\nh\n(e.g., DMSO and DMF) displayed much weaker switching behavior (9.0 and 10.4) (Fig. 3i,\nSupplementary Fig. 51-53). This trend aligned well with the reported plasticization capability\nsequence of PEDOT:PSS additives, where high-δ additives enhance film stretchability by\nh\ndisrupting interchain PSS interactions through hydrogen bonding (Supplementary Table 6)2,\n3; (Line 10-19, Page 17 in the revised Supplementary Information)\nComment 8\nThe Introduction is overly long. Please streamline it by focusing on the key advances of this\nwork; move detailed technical descriptions to the Results & Discussion.\nResponse:\nThank you for your suggestion. We have modified the Introduction section for improved clarity\nand conciseness in the revised manuscript.\nRevision:\n1. However, most conventional electronic devices struggle to replicate the intrinsic\nreconfigurability and responsiveness of biological living tissues at the hardware level5-7.\n(Line 4-6, Page 2 in the revised main manuscript)\n2. In contrast, traditional electronics are typically incapable of reconfiguring their circuitry once\nfabricated, resulting into limited functional plasticity across spatial and temporal dimensions.\n(Line 9-11, Page 2 in the revised main manuscript)\n3. Unfortunately, these two strategies struggled to integrate reconfigurability with excellent\nelectrical performance and size scalability, inferior to bulky but delicate living organisms.\n(Line 13-15, Page 3 in the revised main manuscript)\n4. By leveraging specific ion effect, the conductive network could be finely engineered,\neither locally or globally, to transition among different thermodynamic states with different\nnanophase structures, driven by the delicate balance of inter- and intra-molecular non-\ncovalent interactions of polymers (Fig. 1b). The unique capability enabled controlled spatial\nmodulation of electrical conductivity within a single system over a remarkable range of 4-5\norders of magnitude, without compromising structural integrity and mechanical robustness\n50\n(Fig. 1c-e). (Line 31-35, Page 3, Line 1-2, Page 4 in the revised main manuscript)\n5. In the in-situ wet soldering, the Rec-CN could be directly joined to diverse substrates via\nlaser process or thermal treatment, while preserving its multichannel electrical connections\nand 3-dimensional (3D) geometric integrity, standing in contrast to previously reported\nhydrogel soldering methods which typically required intricate manual operation or were\nincompatible with 3D gels (Fig. 1f, g)23. (Line 4-8, Page 4 in the revised main manuscript)\n6. As a whole, we propose a reversible nanophase regulation strategy to address a critical\nmethodology gap in bridging the spatial scales for the in-situ regulation of electrical\nperformance in reconfigurable electronics. As a result, this approach successfully integrates\ngood electrical and mechanical performance with outstanding reconfigurability features,\nsuch as micro-patternability and re-writability of conductive pathways, in-situ wet\nsolderability with good spatial resolution, and closed-loop recyclability. (Line 14-19, Page\n4 in the revised main manuscript)\nComment 9\nIn the device demonstrations, long-term stability may be compromised by solvent evaporation\nand sensitivity to environmental ions. Please comment on operational lifetimes.\nResponse:\nWe first evaluated the environmental stability of the CP-PVA organogels in terms of mass,\nmechanical robustness, and electrical performance. The organogels exhibited excellent stability\nacross a wide temperature range (25–50 °C, relative humidity: 50 %), as evidenced by\nnegligible changes in mass, mechanical properties, and electrical conductivity after at least one\nweek of exposure under these conditions (Figure R34). However, further increasing the\ntemperature beyond 60 °C led to long-term instability of the organogels, as gradual dehydration\nand microstructural degradation occurred under sustained high-temperature exposure.\nAs a demonstration, the stability of the CP-PVA organogel-based electronic wrist for\nsurface electromyography (sEMG) recording was evaluated after one week of exposure to\nenvironments with relative humidity levels of approximately 20% and 70% at room temperature,\nrespectively. The results showed that the device remained fully functional after exposure, and\nthe recorded sEMG signals exhibited consistent signal-to-noise (~21dB), confirming its reliable\nperformance under both high- and low-humidity conditions (Figure R35).\nAt last, regarding ionic stability, the CP-PVA organogels were expectedly sensitive to ions,\nespecially kosmotropic cations, as elaborated in this work. This limitation is intrinsic to the ion-\nspecific mechanism that underlies the organogel’s phase reconfigurability. A potential strategy\nto mitigate this issue involves encapsulating the organogels with detachable ion-selective\nbarrier materials after fabrication, which will be explored in future studies.\nRevision:\n1. At last, the CP-PVA organogels exhibited higher resistance to environmental humidity and\nhigh/low temperature than their hydrogel counterpart with only water as the dispersed\nmedium, due to the low volatility of glycerol (Supplementary Figs. 12-20 and Supplementary\nNote 5). For example, upon exposure to a high-temperature environment of 80 °C, the CP-\n(Line 14-18, Page 7 in the revised main manuscript)\n2. Supplementary Note 5 | Environmental stability of CP-PVA organogels.\nCompared with hydrogels, glycerol-based organogels demonstrated excellent stability in\nambient environments and high resistance to high temperatures (40-80 °C), greatly boosting\nthe reliability and temperature window of the gel system. As controls, conductive hydrogels\nwere prepared by dialyzing the conductive organogels in water, followed by drying at 80 °C\nand reswelling in purified water. The hydrogels dehydrated quickly even at a mild\ntemperature of 40 °C, as revealed by a sharp loss of ~ 92% in weight within 4 hours,\naccompanied by embrittlement with increased Young’s modulus (Supplementary Fig. 12-14).\nBy contrast, the glycerol-based organogels remain nearly stable at high temperatures up to\n80 °C at different humidity (e.g., 15% and 45%) (Supplementary Fig. 15-19). For example,\nafter exposure to a high-temperature environment (80 °C) with low humidity (15%) for 7\nhours, the organogels experienced slight dehydration (weight loss: 11.4%), with small\ndecreases of 9.5% and 19% in resistance and fracture strain (644% to 522%), respectively.\n(Line 1-13, Page 16 in the revised Supplementary Information)\n3. At last, given the ion-specific mechanism that underlies the organogel’s phase\nreconfigurability, the CP-PVA organogel-based circuit board were expected sensitive to ions,\nespecially kosmotropic cations. A potential strategy to mitigate this issue involves\nencapsulating the organogels with detachable ion-selective barrier materials after fabrication,\nwhich will be explored in future studies. (Line 12-17, Page 21 in the revised main\nmanuscript)\nFigure R34 (Fig. 20 in the revised Supplementary Information). a, b Time-dependent\nchanges in weight (Wₜ/W₀) (a), resistance (Rₜ/R₀) (a), and tensile stress-strain curves (b) of CP-\nPVA organogel subjected to ~50% RH at 50 °C. The stress-strain curves were recorded at a\nstrain rate of 200% min−1. Data in panels a are presented as mean values ± standard deviation\n(s.d.), with four different samples examined in independent measurements.\none week at two different relative humidity levels (20% and 70%) for three weeks. a, b,\nSurface\nelectromyography (sEMG) signals (a) recorded during the gesture performance (gestures III)\nand the corresponding signal-to-noise ratio (SNR) (b). The data in panel b are presented in box-\nand-whisker plots, where the central dots, lines, and box limits indicate the mean, the median,\nand the upper/lower quartiles, and the whiskers extend to 1.5× the interquartile range from the\nquartiles. Statistical significance was assessed using ANOVA for comparisons among multiple\ngroups (panel b), with significance levels denoted as p ≥ 0.05 (not significant, NS), p < 0.05(*),\np < 0.01(**), and p < 0.001(***).\n(Black italic: Reviewer’s remarks; Blue: Our response)\nReviewer #1 (Remarks to the Author):\nThe authors have thoroughly addressed all major and minor comments from the previous review.\nThe revised manuscript now demonstrates improved clarity, well-organized figures, and\nstrengthened validation of both material performance and biomedical applicability. The\nresponses and additional experiments substantially enhance the scientific soundness and\npresentation quality. I am satisfied with the revision and recommend acceptance in its current\nform.\nResponse:\nThank you for your positive recommendation. We greatly appreciate your previous\nconstructive comments, which have significantly improved the quality of the manuscript.\nReviewer #2 (Remarks to the Author):\nMy comments, proposed corrections and additional data requests have been carefully\naddressed.I recommend the article for publication.\nResponse:\nWe sincerely thank you for the careful evaluation and positive assessment of our manuscript.\nReviewer #3 (Remarks to the Author):\nThe authors have addressed all the comments raised in the previous round of review. This\nmanuscript is now ready to be accepted for publication.\nResponse:\nThank you for your thorough review and recommendation. The reviewer’s insightful comments\nand suggestions have been invaluable in strengthening this work and deepening our\nfundamental understanding of the system’s reconfiguration mechanism."}, {"round": 2, "reviewer_comments": {"reviewer_1": "The authors have thoroughly addressed all major and minor comments from the previous review. The revised manuscript now demonstrates improved clarity, well-organized figures, and strengthened validation of both material performance and biomedical applicability. The responses and additional experiments substantially enhance the scientific soundness and presentation quality. I am satisfied with the revision and recommend acceptance in its current form.", "reviewer_2": "My comments, proposed corrections and additional data requests have been carefully addressed.\nI recommend the article for publication.", "reviewer_3": "The authors have addressed all the comments raised in the previous round of review. This manuscript is now ready to be accepted for publication."}, "author_response": ""}]

Decision letter