Titanium dioxide ceramic coatings have been used as catalysts in green technologies for water treatment. However, without the presence of a dopant, its photocatalytic activity is limited to the ultraviolet radiation region. The photocatalytic activity and the structural characteristics of undoped and sulfur-doped TiO2 films grown at 400 ??C by metallorganic chemical vapor deposition (MOCVD) were studied. The photocatalytic behavior of the films was evaluated by methyl orange dye degradation under visible light. The results suggested the substitution of Ti4+ cations by S6+ ions into TiO2 structure of the doped samples. SO4 2??? groups were observed on the surface. S-TiO2 film exhibited good photocatalytic activity under visible light irradiation, and the luminous intensity strongly influences the photocatalytic behavior of the S-TiO2 films. The results supported the idea that the sulfur-doped TiO2 films grown by MOCVD may be promising catalysts for water treatment under sunlight or visible light bulbs.