Toxic pollutants such as diclofenac (DCF) and cadmium(II) have been detected together in various water sources; these compounds have adverse effects on human health. The objective of the present study was to investigate the sorption of DCF and Cd(II) from aqueous solutions on an organobentonite. The organobentonite was synthesized by adsorbing the surfactant hexadecyltrimethylammonium (HDTMA) on bentonite; this was designated OBHDTMA. The sorption of DCF and Cd(II) on OBHDTMA and of Cd(II) on OBHDTMA saturated with DCF (OBHDTMA-DCF) were then studied. The bentonite, OBHDTMA, and OBHDTMA-DCF were characterized by X-ray diffraction, thermogravimetric analysis, and Fourier-transform infrared spectroscopy. The capacity of OBHDTMA for adsorbing DCF depended on the solution pH, ionic strength, and temperature. The effect of pH on the adsorption capacity of OBHDTMA was anomalous because, depending on the concentration of DCF at equilibrium, the adsorption capacity increased or decreased by raising the pH. The capacity of OBHDTMA was enhanced by increasing the temperature from 15 to 35°C and by reducing the ionic strength from 1 to 0.01 N. The dependence of the adsorption capacity on the operating conditions was explained by considering the interactions between the DCF in solution and the surface of OBHDTMA. The maximum sorption capacity of the OBHDTMA for DCF was 388 mg/g at T = 25°C and at pH = 7 and was comparable to those of carbon materials. The adsorption of DCF on OBHDTMA was scarcely reversible, but the desorption percentage increased with pH. The adsorption of DCF on OBHDTMA was due to partition and electrostatic attraction. More Cd(II) was adsorbed on OBHDTMA-DCF than on OBHDTMA and this was influenced by the loading of DCF on the OBHDTMA-DCF. The OBHDTMA-DCF may be used to remove Cd(II) from water solution.