The sorption of uranium and thorium from their aqueous solutions by using 8-hydroxyquinoline modified Na-bentonite (HQ-bentonite) was investigated by the batch technique. Na-bentonite and HQ-bentonite were characterized by X-ray fluorescence (XRF), X-ray diffraction (XRD), scanning electron microscopy (SEM), and Fourier Transform Infrared (FTIR) spectroscopy. Factors that influence the sorption of uranium and thorium onto HQ-bentonite such as solution pH, contact time, initial metal ions concentration, HQ-bentonite mass, and temperature were tested. Sorption experiments were expressed by Freundlich and Langmuir isotherms and the sorption results demonstrated that the sorption of uranium and thorium onto HQ-bentonite correlated better with the Langmuir isotherm than the Freundlich isotherm. Kinetics studies showed that the sorption followed the pseudo-second-order kinetic model. Thermodynamic parameters such as ΔH°, ΔS°, and ΔG° indicated that the sorption of uranium and thorium onto HQ-bentonite was endothermic, feasible, spontaneous, and physical in nature. The maximum adsorption capacities of HQ-bentonite were calculated from the Langmuir isotherm at 303 K and were found to be 63.90 and 65.44 for U(VI) and Th(IV) metal ions, respectively.