Two different organophilic bentonites obtained by cationic exchange with benzyldimethyloctadecylammonium chloride and trimethyloctadecylammonium chloride have been used to adsorb the organic fraction of a tannery sludge. The exchange process was carried out to different extents to obtain bentonite samples with different organophilicities and different interlayer spacings. Before adsorption, the organic matter was extracted by contacting the sludge with a Ca(OH)2 saturated solution. The adsorption capacity was found to increase with the amount of ammonium salt exchanged for both bentonites, but the one exchanged with benzyldimethyloctadecylammonium chloride proved to be more active: up to about 80% TOC could be removed from the contacting solution. The adsorption of the organic matter caused a further increase of the bentonite interlayer spacing. In both cases, the adsorption isotherms were found to be of cooperative type, due to weak adsorbent-adsorbate interactions at low loading followed by increasing adsorbate-adsorbate interactions at increasing loading. The results may be applied to tannery sludge stabilization by cementitious systems.