Modification of Jordanian diatomitaceous clay by aluminum chloride followed by treatment with cationic surfactants was carried out to enhance its capacity to remove phenols and its derivatives as organic pollutants from their aqueous solutions. The original sample and the modified derivatives were thoroughly characterized to check for the modification process by X-ray diffraction, X-ray fluorescence, scanning electron microscopy, total organic carbon, and Fourier transform infrared spectroscopy. The surface area for all studied samples was also estimated using methylene blue method. Experiments were performed to study the role of modified diatomite and surfactants treated modified diatomite samples in the removal of phenol, 4-chlorophenol, and 4-nitrophenol from their aqueous solutions. The results has revealed, in general, that efficiency of diatomite to remove organic pollutants form aqueous solution is higher than efficiency of the unmodified ones, and the efficiency of the treated modified diatomite samples are higher than the untreated samples.