Sorption of four heavy metals (Pb, Cd, Zn and Hg) to calcium bentonite (Ca bentonite), hexadecyltrimethylammonium bentonite (HDTMA bentonite) and benzyltriethylammonium bentonite (BTEA bentonite) was measured as a function of the quaternary ammonium cation (QAC) loading at 25, 50 and 100% of the clay's cation-exchange capacity (CEC). The effects of pH on the surface charge of the clays and heavy metal sorption were also measured. Sorption of Cd, Pb, and Zn was non-linear and sorption of all three metals by HDTMA and BTEA bentonites decreased as the QAC loading increased from 25 to 100%. In most cases, sorption of these metals to 25% BTEA and 25% HDTMA bentonite was similar to or greater than sorption to Ca bentonite. Hg sorption was linear for both HDTMA and BTEA bentonite. No significant effect on Hg sorption was observed with increasing QAC loading on BTEA bentonite. However, an increase of Hg sorption was detected with increasing QAC loading on HDTMA bentonite. This behavior suggests that a process different than cation exchange was the predominant Hg sorption mechanism. Cd, Pb, and Zn sorption decreased with pH. However, this effect was stronger for Cd and Pb than Zn. Hg sorption varied inversely with pH. QAC loading affected the surface charge of the clays. Twenty-five and 50% loading of BTEA cations increased the negative charge on the clay's surface relative to the untreated clay, without affecting the zero point of charge (ZPC) of the clay. Increased QAC loading on HDTMA bentonite causes the surface charge to become more positive and the ZPC increased. One hundred percent of HDTMA bentonite maintained a positive surface charge over the range of pH values tested. The organoclays studied have considerable capacity for heavy metal sorption. Given that prior studies have demonstrated the strong sorption capacity of organoclays for nonionic organic pollutants, it is likely that organoclays can be useful sorbents for the treatment of effluent streams containing both organic contaminants and heavy metals.