The ZnO/TiO2 composite films were deposited over glass using spin coating technique by sol-gel process. Single-walled carbon nanotubes (SWNTs) were used to modify the ZnO/TiO2 films successfully in this paper. The structure and composition of the ZnO/TiO2 composite and SWNTs doped ZnO/TiO2 composite were characterized by X-ray diffraction (XRD). The morphology of samples was characterized by scanning electron microscopy (SEM). The photocatalytic activity was investigated by photocatalytic degradation of aqueous methyl orange under ultraviolet (UV) radiation. The UV-vis absorption spectra of the ZnO/TiO2 films and SWNTs doped ZnO/TiO2 films in the wavelength region 200~800 nm were obtained. The results indicate that the SWNTs addition can decrease the grain size of ZnO/TiO2, which can enhance the photocatalytic activity. UV-vis absorption spectra of SWNTs-ZnO/TiO2 showed obvious blue shifts compared with ZnO/TiO2. The optimal amount of doping SWNTs is 1% according to this research. The enhanced mechanism of the SWNTs for the photocatalytic activity in ZnO/TiO2 films was analyzed in this article.