Polyacrylonitrile (PAN) and bentonite (B)/zeolite (Z)-PAN composites were prepared by direct polymerization of acrylonitrile (AN) and AN adsorbed onto B and Z. PAN and the composites were subjected to amidoximation procedure to obtain polyacrylamidoxime (PAO), B-PAO and Z-PAO compositions. The structural features were evaluated by FT-IR, XRD and SEM analysis. The adsorption dependency of the materials on ion concentration, temperature and time were investigated for Pb2+ and UO2 (2+). The adsorption capacities of B/Z-PAO composites were higher than those of pure PAO. The values of enthalpy and entropy changes were positive. The kinetics of the adsorption was well defined by the pseudo second order rate model. For the use of 1 M HCl as a regenerative effluent, the composites were reusable for five sequential treatments without any change in their structures whereas PAO completely gelled in the first use.