We have examined the photoinduced hydrophilicity of SiO x :OH/TiO 2 multilayer films containing a high degree of Si-OH bonding. The ultrahydrophilic properties were observed under UV irradiation of 10 mW/cm 2 , and a technique for preserving these changes in the dark has been successfully developed. Different thicknesses of SiO x :OH films were deposited onto photocatalytic TiO 2 layers in an Ar/H 2 O ambient by DC reactive magnetron sputtering. The deposited structures were analyzed by secondary ion mass spectroscopy (SIMS), Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), and scanning electron microscopy (SEM), and their hydrophilic properties were evaluated by contactangle measurement with respect to purified wafer. Cross sections of the structure of the SiO x :OH/TiO 2 multilayer films show that SiO x :OH is deposited on the columnar-structured TiO 2 film in a discontinuous manner. The amount of hydrogen in the SiO x :OH film depends on the H 2 O partial pressure, and the concentration depends heavily on the presence of Si-OH. The SiO x :OH/TiO 2 multilayer films exhibit hydrophilic properties, even without any UV irradiation, and the hydrophilic properties under photoexcitation are also improved. The presence of -OH groups in the SiO x :OH films is considered to have an effect on this improvement in hydrophilicity.