Abstract: New pillared clay-based adsorbents have been prepared by incorporating a nonionic surfactant of general formula C12–29H25–29O(CH2CH2O)5H (commercial name, Tergitol 15S-5), during the synthesis of the aluminum hydroxide pillaring reagent. Different loadings of surfactant have been examined. The presence of the surfactant enhanced the adsorption capacity of the clay toward 3-monochlorophenol from aqueous solution. On the basis of adsorption results for a series of clays with increasing surfactant loadings, the best adsorbent was obtained at a surfactant loading of 255 mg/g of clay. At this loading, the surfactant occupies the micropores, as well as the mesopores and the external surfaces of the pillared clay. Analysis of the adsorption isotherms for 3-monochlorophenol, 3,5-dichlorophenol, 3,4,5-trichlorophenol and pentachlorophenol at different pH shows that the most energetic adsorption sites are the surfactant-occupied micropores between pillars. Additional binding of chlorinated phenols occurs at surfactant sites on external surfaces and mesopores. Upon calcination at 500°C, the clay is converted to a conventional alumina-pillared clay with a basal spacing near 16 Å. This calcined product can be reused as an adsorbent for chlorinated phenols by readsorbing fresh surfactant. The recycled adsorbent exhibits performance properties comparable to the original adsorbent. These results demonstrate the feasibility of utilizing a surfactant-modified pillared clay as a recyclable adsorbent and combustion catalyst for environmental pollutants.