Carbon and nitrogen species‐involved TiO2 (CN‐TiO2) were systematically synthesized by thermal condensation of cyanuric acid on the TiO2 surface. And the photocatalytic reactions for H2 production from sacrificial aqueous solutions were performed on several CN‐TiO2 photocatalyst under visible‐light irradiation. The photocatalytic activity of the CN‐TiO2 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‐TiO2 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 H2 production is associated with effective charge separation under photo‐ excitation of highly dispersed carbon nitride on the TiO2 surface.