C-N-co-doped anatase TiO 2 photocatalysts were successfully prepared by a sol-gel method and characterized by Brunauer-Emmett-Teller method, X-ray diffraction, UV-Vis diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscope (SEM), and surface photovoltage spectroscopy (SPS). The separation efficiency of photogenerated charges was investigated using benzoquinone as scavenger. An obvious redshift of the absorption edge of TiO 2 was observed owing to C and N doping. Moreover, doping C and N into TiO 2 increases the content of hydroxyl content on the surface of photocatalysts and photoinduced charge separation efficiency. The photocatalytic activity was evaluated by decolorization of methyl orange (MO) aqueous solution under simulated sun light and visible light irradiation. The results show that photocatalytic activities of the TiO 2 are greatly improved by C and N co-doping, which can be further confirmed by the removal of COD of MO aqueous solution. Graphical Abstract In general, the strong SPS response corresponds to the high separation rate of photoinduced charge carriers on the basis of the SPS principle. Thus, it can be confirmed that the C-, N-TiO 2 sample has a higher charge separation rate than the pure TiO 2 sample, and the 4 % C-, N-TiO 2 shows the highest charge separation rate 400 420 440 460 480 500 0.00 0.02 0.04 0.06 Photovoltage (mV) Wavelength (nm) 5%C-,N-TiO 2 0%C-,N-TiO 2 4%C-,N-TiO 2 300 350 400 450 500 -0.5 0.0 0.5 1.0 1.5 2.0 2.5 3.0