Abstract Carbon and nitrogen species‐involved TiO 2 ( CN‐TiO 2 ) were systematically synthesized by thermal condensation of cyanuric acid on the TiO 2 surface. And the photocatalytic reactions for H 2 production from sacrificial aqueous solutions were performed on several CN‐TiO 2 photocatalyst under visible‐light irradiation. The photocatalytic activity of the CN‐TiO 2 was influenced by total amounts of carbon and nitrogen species, and the preferable activity was ten times higher than that of pristine carbon nitride. Here, the states of the CN‐TiO 2 photocatalyst were characterized by XPS , FT‐IR and UV –vis spectroscopy as well as DFT calculations. The photo‐electrochemical measurements confirmed that the enhancement of H 2 production is associated with effective charge separation under photo‐ excitation of highly dispersed carbon nitride on the TiO 2 surface.