A method of forming an electrode for capacitive deionization includes depositing an slurry onto a substrate, wherein the slurry comprises a porous material, a first crosslinkable hydrophilic polymer, and a crosslinker for the first crosslinkable hydrophilic polymer; annealing the slurry deposited on the substrate to create a crosslinked porous layer on the substrate; depositing an solution comprising an ion-exchange material, a second crosslinkable hydrophilic polymer, and a crosslinker for the second crosslinkable hydrophilic polymer onto the crosslinked porous layer; and optionally annealing and/or drying the solution on the crosslinked porous layer.