The natural bentonite (BC) and kaolinite (KC) were modified with two surfactant of hexadecyltrimethylammonium bromide (HDTMA) and phenyltrimethylammonium bromide (PTMA) to form four kinds of organic-modified clays, i.e., HDTMA-bentonite (BHM), HDTMA-kaolinite (KHM), PTMA-bentonite (KPM) and PTMA-kaolinite (KPM). The modified minerals were characterized by X-ray fluorescence (XRF), X-ray diffraction (XRD) and FT-IR spectroscopy. The surface areas were determined using methylene blue adsorption method. Cation-exchange capacity (CEC) was estimated using an ethylenediamine complex of copper method and the modifier loading was calculated from the total carbon analysis. The ability of raw and organo-modified clays to remove phenol from aqueous solutions has been carried out as a function of contact time, pH and temperatures using a batch technique. The removal of phenol from aqueous solutions by modified clays seems to be more effective than unmodified samples. The adsorption capacity was found to increase with increasing temperature indication that the adsorptions were endothermic. The adsorption of phenol onto these clays was found to be increased by increasing of pH value and the adsorption patterns data are correlated well by Langmuir and Freundlich isotherm models and that the adsorption is physical in nature. The experimental data fitted very well with the pseudo-second-order kinetic model. The thermodynamic study of adsorption process showed that the adsorption of phenol with these six adsorbents was carried out spontaneously, and the process was endothermic in nature.