Sorption properties of Greek bentonites and zeolites were investigated in raw form and after irradiation for removal of Cs, Co and Eu from aqueous solutions using 137Cs, 60Co and 152Eu as tracers and γ-spectroscopy. The sorption experiments were undertaken under different conditions (pH, concentration, competitive ions and temperature). The structural changes of the sorbents due to irradiation and metal sorption were examined through XRD, FTIR and SEM/EDS. Sorption isotherms were reproduced by mathematical models and thermodynamic parameters were derived. The results showed that the sorption capacity was slightly affected by irradiation. The environmental compatibility tests proved the safe disposal of the investigated materials.