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Nanocrystalline TiO₂ films used for gas sensors have been studied by means of surface photovoltage spectroscopy and other analytical tools to investigate the oxygen chemisorption effect on the electrical properties of the films. The results show that the surface (and intergranular interface) band bending increases with oxygen exposure due to electron trapping at midgap states induced by chemisorption. The surface electronic structure is revealed by the measurements, allowing determination of the sensing mechanism of these important films. In addition, a photoinduced chemisorption of oxygen at room temperature is observed. This has important implications for low-temperature gas sensors.