The sorption of benzene to bentonite, activated carbon, and two organo-clays synthesized with the quaternary ammonium organic cations hexadecyltrimethylammonium (HDTMA) and benzyltriethylammonium (BTEA) was quantified as a function of total organic carbon content. The unmodified bentonite sorbed no benzene, while the activated carbon exhibited the strongest benzene uptake. For the organoclays, organic cations were exchanged onto Wyoming bentonite at four different percentages of the clay's cation exchange capacity. For HDTMA clay, in which partitioning is the dominant sorptive medium, it was determined that benzene sorption increased as the total organic carbon content increased (as the clay became more hydrophobic). In contrast, the sorption of benzene to BTEA clay, an adsorptive clay, decreased as the total organic carbon content of the clay was increased. It is believed that the sorptive capacity of BTEA clay decreases due to the formation of positively charged dimers on the clay's surface that block access to the sorptive sites. The organoclays sorbed more benzene than the unmodified bentonite, but less than the activated carbon.