Clay-based adsorbents were synthesized by incorporating anionic surfactants, sodium octylsulfate (SOS), sodium dodecylsulfate (SDS), sodium 4-octylbenzenesulfonate (SOBS), and sodium dodecylbenzenesulfonate (SDBS), into magnesium aluminum layered double hydroxide (Mg-Al LDH) via ion exchange. Adsorption isotherms indicated the amount of surfactants intercalated decreased in the order: SDS>SOBS>SDBS>SOS. X-ray diffraction analysis of the organo-LDHs revealed that surfactant molecules could adopt various configurations within the Mg-Al LDH interlayer space, with SOS forming bilayers whereas others exhibited monolayer arrangements. Intercalation of surfactants into Mg-Al LDH resulted in a decrease in surface area as determined by BET analysis. The products were also examined for their ability to adsorb organic pollutants. The adsorption results indicated that both 1,2,4-trichlorobenzene and 1,1,1-trichloroethane could be adsorbed by all of the organo-LDHs studied, presumably due to partitioning, with adsorption affinity dependent upon the type of surfactant used. Adsorption results indicated anionic surfactants intercalated into Mg-Al LDH form a more effective partition phase than octanol.