Visible light-responsive TiO2 (Vis-TiO2) thin films were successfully developed by a radio-frequency (RF) magnetron sputtering deposition method. These Vis-TiO2 thin films exhibited a declined composition of the O/Ti ratio from the surface (O/Ti = 2.00) to bottom (O/Ti = 1.93), enabling the absorption of visible light. Pt-loaded Vis-TiO2 was, thus, found to decompose water involving methanol or a 0.05 M silver nitrate Solution under visible light irradiation.