The removal of chromates and iodides from aqueous solutions by organo-modified tuffs from the Pentolofos area (Thrace, Greece) was investigated using (51)Cr- and (131)I-labelled solutions and gamma-ray spectroscopy. The zeolitic material was modified by hexadecyltrimethyl-ammonium bromide (HDTMA-Br) and octadecyltrimethyl-ammonium bromide (ODTMA-Br) and characterized by scanning electron microscopy, FT-IR spectrometry and zeta potential measurements. Both experimental study and modelling indicated that both organo-zeolitic sorbents have a bigger affinity for iodide than for chromate. The chromium uptake did not seem to be influenced by the type of modifier but showed, as expected, a dependence on the solution pH. The maximum sorption capacity (2.27 mg/g) of Cr(VI) was achieved for the solution of initial pH 4. On the other hand, the HDTMA-modified tuff showed a lower sorption affinity for iodides than did the ODTMA-modified one (3.37 and 4.02 mg/g, respectively).