This study concerns the adsorption properties of organo-bentonites obtained through the modification performed at 25%, 50% and 100% of the cation exchange capacity (CEC) using tetradecyl trimethylammonium bromide (TDTAB) and hexadecyl trimethylammonium bromide (HDTAB). According to the XRD measurements, TDTAB and HDTAB form bilayers between the silicate layers when the montmorillonite surface is modified by 100% CEC. At 25% and 50% CEC, a random interstratification of monolayer and bilayer structures is observed. The surface area of bentonite decreases upon modification. The adsorption proper-ties of organo-bentonites were tested using phenol as a model pollutant. Batch kinetic and isotherm studies were conducted over the concentration range from 50 to 1000 ppm at pH of 5.5. The adsorption excess isotherms of bentonites show different regions. A considerable increase was observed in the adsorption efficiency of montmorillonite modified with HDTAB at 100% CEC. (C) 2004 Elsevier B.V. All rights reserved.