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A radio-frequency magnetron sputtering (RF-MS) deposition method was applied to prepare a unique double-layered visible light-responsive TiO 2 thin film photocatalyst on a Ti foil substrate (DL-TiO 2 /Ti). The DL-TiO 2 /Ti consists of a UV light-responsive TiO 2 thin film (UV-TiO 2 ) deposited as the inner block layer on a Ti foil substrate and a visible light-responsive TiO 2 thin film (Vis-TiO 2 ) deposited as the outer layer. DL-TiO 2 /Ti exhibited higher photoelectrochemical and photocatalytic performance under both UV and visible light irradiation than a single-layered Vis-TiO 2 thin film photocatalyst deposited on a Ti foil substrate. The optimal thickness of the UV-TiO 2 film as the inner block layer of DL-TiO 2 /Ti was found be 100 nm in terms of the photoelectrochemical and photocatalytic performance. Expanding on this work, a novel double-layered TiO 2 thin film device, DL-TiO 2 /Ti/ Pt, was also prepared by the RF-MS method where DL-TiO 2 was deposited on one side of a Ti foil substrate and Pt was deposited on the other side. The separate evolution of H 2 and O 2 from H 2 O was successfully achieved by using an H-type glass cell consisting of two aqueous phases separated by the DL-TiO 2 /Ti/Pt and a protonexchange membrane. The separate evolution rate of H 2 and O 2 was found to be dramatically enhanced on DL-TiO 2 /Ti/ Pt as compared with a single-layered Vis-TiO 2 thin film device under white light irradiation from a solar simulator.Keywords Photocatalytic water splitting Á TiO 2 photocatalyst Á Separate evolution of H 2 and O 2 Á Visible light Á Double-layered thin film

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