A visible-light-active nitrogen and gadolinium codoped TiO2 catalyst was synthesized by the sol-gel route. For comparison, Gd-doped sample, N-doped sample, and pure titania were prepared through the same method, without adding the corresponding dopants. The as-prepared photocatalysts were characterized by X-ray diffraction (XRD) and Uv-vis spectra. The results showed that the codoped photocatalyst exhibited a smaller size than the undoped titania. The transformation from anatase to rutile was suppressed by doping with N and Gd atoms. Furthermore, the absorbance spectra of N, Gd-codoped TiO2 exhibited a significant red shift to the visible region. The photocatalytic activity of N, Gd-codoped TiO2 was evaluated by photodegradation of methyl orange under visible light irradiation. This codoped sample exhibited enhanced photocatalytic activity compared to N-doped TiO2, Gd-doped TiO2, and pure TiO2. The improvement of the photocatalytic activity was ascribed to the synergistic effects of the N and Gd co-doping.