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Titanium-substituted hydroxyapatite (Ti-HAp) is a potential photocatalyst with high adsorption capability for organic compounds. As described herein, the surface of Ti-HAp was modified by WOx. Photocatalytic decomposition activity on gaseous 2-propanol was increased by seven times by the modification. Little difference was obtained in the crystalline phase, specific surface area, and the light absorption edge between before and after the modification. However, photoluminescence emission intensity by UV irradiation was decreased by the modification. Results show that UV irradiation changed the valence number ratio of W cations under N2 atmosphere. Furthermore, first-principles simulations of molecular dynamics and electronic structure suggest that carrier separation is promoted by WOx clusters acting as a co-catalyst and suggest that those photoexcited electrons can be consumed by atmospheric oxygen. These experimental and theoretical investigations have demonstrated clearly that the photoexcited electrons can transfer from a Ti-hybridized band in Ti-HAp to WOx, thereby promoting charge separation.