A number of both UV and thermally radically induced cross-linked epoxy acrylates and vinyl polymers/copolymers (cross-linked with divinyl benzene) have been prepared and predoped with different charge-transport media (CTM) and examined as alternative potential durable wear resistant charge-transport layers (CTL) for electrophotographic applications. The CTMs studied were tri- p-tolylamine (TpTA), 2,5-bis(4-diethylaminophenyl-1,3,4-oxadiazole) (OXD), p-diethylaminobenzaldehyde-diphenylhydrazone (DEH) and p-diethylaminophenyl benzaldehyde methylphenyl hydrazone (T191). The polymer binders were based on epoxy acrylates, epoxy resins (amine cured) and divinyl benzene cross-linked styrene/styrene- co-methyl methacrylate, styrene—allyl methacrylate and poly(vinyl cinnamate) and compared with the properties of a conventional polycarbonate CTL. The structure of the cross-linked polymer, nature of the CTM and its concentration controlled the extent of cross-linking and mobility of charge within the coating. UV cured systems were found to fail as CTLs due to the presence of high levels of hydroxy groups on the polymer backbone, residual initiators and photosensitivity and photolysis products of the CTM's trapping and inhibiting charge migration. Polymers containing styrene units, on the other hand, display good charge transport properties compared with polycarbonate due to strong interactions of the pendant phenyl groups stabilising the cation radicals produced on illumination. However, these coatings, although hard were found to be brittle in nature. Copolymerisation with methyl or allyl methacrylate reduced the brittleness but also the mobility of charge due to spacing of the phenyl rings along the polymer network. Thermal cross-linking of a polymer that undergoes a 2 + 2 cycloaddition, poly(allylcinnamate), gave a hard tough coating that exhibited promise as an effective CTL when compared to that of polycarbonate.