Sm, Zr doped nanocrystalline TiO2 powers were prepared successfully by a facile ultrasonic assisted sol-gel method. The products were characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM), respectively. X-ray diffraction peaks could be assigned to anatase TiO2, which confirms the crystallinity of the as-prepared samples. The SEM images demonstrated that the crystalinity is formed with spherical aggregates with average diameters ranging from 10 to 20 nm. The photocatalytic activity was studied on the photocatalytic degradation of methyl orange (MO) aqueous solution irradiated with UV-visible light. Under UV-visible light irradiation, the photocatalytic performances of the doped samples were much better than that of pure TiO2, and the co-dopant showed highest. It demonstrated that a strong Sm-Zr synergistic interaction might play a decisive role in driving the excellent photocatalytic performance of TiO2.