The ability of poly(N-vinylimidazole) hydrogels to bind Cu(II), Co(II), Ni(II), Zn(II), Cd(II), Pb(II), Hg(II), Na(I) and Ca(II) cations, as well as uranyl, vanadium, rhenium, and molybdenum complexes, was studied by a batch equilibrium procedure using atomic absorption spectroscopy and UV-Vis spectrophotometry. The optimum pH for ion adsorption was determined in any case. The influence of the cross-linking degree of the hydrogel on the sorption kinetics and the sorption capacity at equilibrium were also studied. Sorption from the binary mixture Cu(II) + U(VI) was also analyzed at the optimum pH. Elution of the ions adsorbed from single and binary solutions was achieved in all cases. A selective desorption of loaded hydrogels with two types of ions was attained. The general conclusion is that poly(N-vinylimidazole) hydrogels are excellent materials for retention of all the ions studied here [except for Pb(II), Na(I), and Ca(II)]. The elution, which can be selective, allows regeneration of the hydrogel.