This study investigates the mechanism of photosensitization and the recombination of excited electron-hole pairs affected by depositing platinum (Pt) on the surface of titanium dioxide (TiO 2 ). A new catalyst of Pt-TiO 2 was prepared by a photoreduction process. Being model reactions, the photocatalytic oxidation of methylene blue and methyl orange in aqueous solutions using the Pt-TiO 2 catalyst was carried out under either UV or visible light irradiation. The experimental results indicate that an optimal content of 0.75% Pt-TiO 2 achieves the best photocatalytic performance of methylene blue and methyl orange degradation and that the PtTiO 2 catalyst can be sensitized by visible light. The interaction of Pt and TiO 2 was investigated by means of UV-visible absorption spectra, photoluminescence emission spectra, and X-ray photoelectron emission spectroscopy. The Pt 0 , Pt 2+ and Pt 4+ species existing on the surface of PtTiO 2 , and the Ti 3+ species existing in its lattice may form a defect energy level. The Pt impurities, * Author whom all correspondence should be addressed to This is the Pre-Published Version.2 including Pt, Pt(OH) 2 , and PtO 2, and the defect energy level absorb visible light more efficiently in comparison with the pure TiO 2 and hinder the recombination rate of excited electron/hole pairs.