TiO 2 thin film photocatalysts which can work under visible light irradiation were successfully developed in a single process by applying a RF magnetron sputtering (RF-MS) deposition method. The TiO 2 thin films prepared at higher than 773 K showed efficient absorption of visible light, while the TiO 2 films prepared at around 473 K were highly transparent. This clearly means that the optical properties of these films, which absorb not only UV but also visible light, can be controlled by the preparation conditions using the RF-MS deposition method. These visible light-responsive films were found to exhibit effective photocatalytic reactivity at room temperature for the decomposition of NO and oxidation of acetalydehyde with O 2 . Various characterization studies showed that orderly aligned columnar TiO 2 crystals of ca. 100 nm could be observed only for the visible light-responsive TiO 2 thin films. Such unique structural factors are considered to be essential in modifying the electronic properties of the TiO 2 semiconductors, enabling the efficient absorption of visible light. Moreover, crystalline TiO 2 thin films could be prepared on thermally unstable polycarbonate substrates at 353 K by using this RF-MS deposition method.