A method of printing with water-based inkjet inks on a water-impermeable, low-surface-energy substrate having an initial surface energy of less than 0.05 N/m (50 dyn/cm), wherein the low-surface-energy substrate is selected from polyesters, polyimides, polycarbonates, polystyrenes, polyolefins, polyurethanes, polyvinyl acetates, polyvinyl chlorides, polyvinylidene chlorides, and copolymers, mixtures, co-extrudates, or laminates thereof, comprising: a) modifying surface properties of the water-impermeable, low-surface-energy substrate to increase the surface energy and make it receptive to a water-based coating composition; b) coating the modified surface of the water-impermeable, low-surface-energy substrate with a first layer comprising a colorless and transparent water-based tie-layer composition comprising a polymeric binder that is a polyvinyl alcohol, polyvinyl amine, gelatin, poly(ethyleneimine), epoxy resin, polyurethane, polyacrylamide, a polymer or copolymer comprising 50 to 100 mole % of glycidyl acrylate or glycidyl methacrylate, or a derivative, copolymer, or blend thereof; c) coating over the first layer with a second layer comprising a colorless water-based ink-receptive composition comprising: i) a water-soluble multivalent metal salt wherein at least 0.5 g of the water-soluble multivalent metal salt is capable of dissolving in 100 ml of water at 20°C; and ii) a hydrophilic binder polymer; d) depositing directly on the surface of the second layer one or more water-based ink compositions containing an anionically stabilized pigment colorant, wherein the one or more water-based ink compositions are deposited in a predetermined pattern with an inkjet deposition system in response to electrical signals; e) drying the first and second coated layers and the deposited inks to substantially remove the water, wherein any residual water after the drying process is within the normal ranges that are measured when the dried coated layers are equilibrated at an ambient environment condition of 20°C to 30°C and 20% to 80% relative humidity; and f) post-coating the one or more dried deposited ink layers and any exposed first and second layers with one or more functional compositions to form a multi-layered structure, wherein each of the one or more functional compositions are capable of forming one or more functional layers providing one or more of opacity, protection, and adhesion. a) modifying surface properties of the water-impermeable, low-surface-energy substrate to increase the surface energy and make it receptive to a water-based coating composition; b) coating the modified surface of the water-impermeable, low-surface-energy substrate with a first layer comprising a colorless and transparent water-based tie-layer composition comprising a polymeric binder that is a polyvinyl alcohol, polyvinyl amine, gelatin, poly(ethyleneimine), epoxy resin, polyurethane, polyacrylamide, a polymer or copolymer comprising 50 to 100 mole % of glycidyl acrylate or glycidyl methacrylate, or a derivative, copolymer, or blend thereof; c) coating over the first layer with a second layer comprising a colorless water-based ink-receptive composition comprising: i) a water-soluble multivalent metal salt wherein at least 0.5 g of the water-soluble multivalent metal salt is capable of dissolving in 100 ml of water at 20°C; and ii) a hydrophilic binder polymer; i) a water-soluble multivalent metal salt wherein at least 0.5 g of the water-soluble multivalent metal salt is capable of dissolving in 100 ml of water at 20°C; and ii) a hydrophilic binder polymer; d) depositing directly on the surface of the second layer one or more water-based ink compositions containing an anionically stabilized pigment colorant, wherein the one or more water-based ink compositions are deposited in a predetermined pattern with an inkjet deposition system in response to electrical signals; e) drying the first and second coated layers and the deposited inks to substantially remove the water, wherein any residual water after the drying process is within the normal ranges that are measured when the dried coated layers are equilibrated at an ambient environment condition of 20°C to 30°C and 20% to 80% relative humidity; and f) post-coating the one or more dried deposited ink layers and any exposed first and second layers with one or more functional compositions to form a multi-layered structure, wherein each of the one or more functional compositions are capable of forming one or more functional layers providing one or more of opacity, protection, and adhesion.