The surface engineering of polycarbonate track-etched (PCTE) membranes was performed to create a permselective membrane for the removal of trace levels of fission products and transuranic metals from acidic streams. Electroless gold deposition was used to place a gold coating on the PCTE substrates. The gold coating was subsequently functionalized through the formation of a self-assembled monolayer of dodecanethiol, which was further functionalized with di-(4-t-butylphenyl)-N, N-diisobutylearbamoylmethylphosphine oxide. Transport characteristics of metal ions, Cs-137, Sr-85, Am-241, and Pu-239, were obtained using a two-compartment diffusion apparatus. Transport studies showed that the functionalized membranes enhance the transport rates of Am-241. and Pu-239 and inhibit the transport of Cs-137 and Sr-85. Diffusion studies over an extended time revealed that the facilitated transport characteristics of Pu-239 through the ligand-coated membranes are dependent on nitrate anion concentrations in the feed and sink cells.