The removal of Cr(VI) from aqueous solutions under various conditions was investigated using a natural clinoptilolite and a synthetic zeolite derived from fly-ash (Na-P1), modified either with hexadecyltrimethylammonium bromide (HDTMA) or octadecyltrimethylammonium bromide (ODTMA). The study was focused mainly on the impact of the properties of the zeolite on the sorption capacity, the sorption mechanism, the influence of pH and the durability of the immobilization. The zeolites were modified with HDTMA and ODTMA surfactants up to 100% and 120% of their external cation exchange capacity. Batch and column studies were conducted to evaluate the influence of pH and the initial Cr(VI) concentration on their efficiencies for removing chromates. The organo-zeolites show a significant ability to remove Cr(VI) from aqueous solutions. The amount of Cr(VI) removed by organo-clinoptilolite and organo-zeolite Na-P1 is greater at low pH values, whereas the sorption efficiency decreased with increasing pH. Sorption of Cr(VI) was more efficient with the HDTMA-modified organo-clinoptilolite (150 mmol Cr(VI)/kg) than the ODTMA-modified clinoptilolite (132 mmol Cr(VI)/kg). The maximum sorption capacity was obtained with the 1.2 × ECEC ODTMA-modified clinoptilolite (237 mmol Cr(VI)/kg). The organo-zeolites Na-P1 adsorbed Cr(VI) from aqueous solutions more effectively and were much more durable than the organo-clinoptilolites.