Visible light-responsive TiO2 (Vis-TiO2) thinfilms were prepared by a radio frequency magnetronsputtering deposition method. The photoelectrochemicalperformance was improved by adding various kinds andconcentrations of alcohol, i.e., model compounds of biomass,to water. The separate evolution of pure H2 wasobserved to proceed efficiently on these Vis-TiO2 thin filmsunder visible light irradiation by using an aqueous solutionof methanol.