A battery electrode composition comprising composite particles, each composite particle comprising: a high-capacity active material provided to store and release ions during battery operation, wherein the active material_comprises (i) F, Cl, Br, S, Se, N, P, H, Fe, Zn, Cd or Ni and exhibits a specific capacity of at least 220 mAh/g as a cathode active material or (ii) Si, Ge, Sn, Al, Pb, An, Mg, Fe, Zn, Cd or Ni and exhibits a specific capacity of at least 400 mAh/g as an anode active material; a porous, electrically-conductive scaffolding matrix material within the pores of which the active material is disposed; and a shell contacting the scaffolding matrix material and at least partially encasing the active material and the scaffolding matrix material, wherein the shell is configured to form a barrier between the active material of each composite particle and an electrolyte solvent, wherein each composite particle exhibits at least one material property that changes from the center to the perimeter of the scaffolding matrix material, and wherein the at least one material property comprises one or more of: (i) a material composition of the active material, the material composition of the active material including a first active material that is more concentrated near the center of the scaffolding matrix material and a second active material that is more concentrated near the perimeter of the scaffolding matrix material, and wherein the first active material has a higher energy density than the second active material, (ii) a concentration of nucleation-inducing defects of the scaffolding matrix material which decreases from the center to the perimeter, (iii) an average pore size of the scaffolding matrix material that is larger near the center of the scaffolding matrix material and the perimeter of the scaffolding matrix material as compared to an intermediate region of the scaffolding matrix material located between the center and the perimeter, (iv) a pore orientation of slit-shaped pores of the scaffolding matrix material, or (v) any combination thereof. a high-capacity active material provided to store and release ions during battery operation, wherein the active material_comprises (i) F, Cl, Br, S, Se, N, P, H, Fe, Zn, Cd or Ni and exhibits a specific capacity of at least 220 mAh/g as a cathode active material or (ii) Si, Ge, Sn, Al, Pb, An, Mg, Fe, Zn, Cd or Ni and exhibits a specific capacity of at least 400 mAh/g as an anode active material; a porous, electrically-conductive scaffolding matrix material within the pores of which the active material is disposed; and a shell contacting the scaffolding matrix material and at least partially encasing the active material and the scaffolding matrix material, wherein the shell is configured to form a barrier between the active material of each composite particle and an electrolyte solvent, wherein each composite particle exhibits at least one material property that changes from the center to the perimeter of the scaffolding matrix material, and wherein the at least one material property comprises one or more of: (i) a material composition of the active material, the material composition of the active material including a first active material that is more concentrated near the center of the scaffolding matrix material and a second active material that is more concentrated near the perimeter of the scaffolding matrix material, and wherein the first active material has a higher energy density than the second active material, (ii) a concentration of nucleation-inducing defects of the scaffolding matrix material which decreases from the center to the perimeter, (iii) an average pore size of the scaffolding matrix material that is larger near the center of the scaffolding matrix material and the perimeter of the scaffolding matrix material as compared to an intermediate region of the scaffolding matrix material located between the center and the perimeter, (iv) a pore orientation of slit-shaped pores of the scaffolding matrix material, or (v) any combination thereof. (i) a material composition of the active material, the material composition of the active material including a first active material that is more concentrated near the center of the scaffolding matrix material and a second active material that is more concentrated near the perimeter of the scaffolding matrix material, and wherein the first active material has a higher energy density than the second active material, (ii) a concentration of nucleation-inducing defects of the scaffolding matrix material which decreases from the center to the perimeter, (iii) an average pore size of the scaffolding matrix material that is larger near the center of the scaffolding matrix material and the perimeter of the scaffolding matrix material as compared to an intermediate region of the scaffolding matrix material located between the center and the perimeter, (iv) a pore orientation of slit-shaped pores of the scaffolding matrix material, or (v) any combination thereof.