A sorbent dialysis cartridge is provided for removal of uremic toxins from dialysate wherein the sorbent cartridges can use non-enzymatic urea-binding materials in place of urease. The cartridge can have a first sorbent layer loaded with a polymerizable urea complexing agent and a second sorbent layer loaded with a crosslinker. The crosslinker can be crosslinkable with a soluble urea complex reaction product of the polymerizable urea complexing agent and urea when passing through the first sorbent layer to form a crosslinked polymeric urea complex which is attachable to the second sorbent layer. In another option, a sorbent layer can be used which has an insolubilized crosslinked polymeric urea-bindable complex attached thereto, wherein the crosslinked polymeric urea-bindable complex can be a reaction product of a crosslinker and polymerizable urea complexing agent. Methods and sorbent dialysis systems using the cartridge, and methods of making the sorbent material, are provided.