TiO 2 thin film photocatalysts which could induce photoreactions under visible light irradiation were successfully developed in a single process by applying an ion engineering technique, i.e., the radio frequency (RF) magnetron sputtering deposition method. The TiO 2 thin films prepared at temperatures greater than 773 K showed the efficient absorption of visible light; on the other hand, the TiO 2 thin films prepared at around 573 K were highly transparent. This clearly means that the optical properties of TiO 2 thin films, which absorb not only UV but also visible light, can be controlled by the preparation temperatures of the RF magnetron sputtering deposition method. These visible light responsive TiO 2 thin films were found to exhibit effective photocatalytic reactivity under visible light irradiation (k [ 450 nm) at 275 K for the reductive decomposition of NO into N 2 and N 2 O. From various characterizations, the orderly aligned columnar TiO 2 crystals could be observed only for the visible light responsive TiO 2 thin films. This unique structural factor is expected to modify the electronic properties of a TiO 2 semiconductor, enabling the efficient absorption of visible light.