The development of visible light-responsive TiO2 (Vis-TiO2) thin films has been achieved by applying a radio-frequencymagnetron sputtering deposition (RF-MS) method. Pt-loaded Vis-TiO2 thin films act as photocatalysts to decompose waterinvolving sacrificial reagent such as methanol or silver nitrate even under visible light (k 3 420 nm) irradiation. It was also foundthat Pt-loaded Vis-TiO2 thin films decompose pure water into H2 and O2 stoichiometrically under light irradiation of wavelengthslonger than 390 nm. Vis-TiO2 thin films exhibit columnar structures perpendicular to the substrate and a declined composition ofthe O/Ti ratio from the surface (O/Ti ¼ 2.00) to bottom (O/Ti ¼ 1.93). This unique structure (anisotropic structure) of Vis-TiO2can be considered an important factor in the modification of the electronic properties of Vis-TiO2 thin films, enabling theabsorption of visible light. Furthermore, the effect of the Pt loadings on the photocatalytic activity of the TiO2 thin films wasinvestigated and the optimum Pt loading was determined to be 21 lg/cm2 as Pt metal.