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Activation of metal oxides by light is a robust yet facile approach to manipulating their surface chemistry for favorable reactions with target molecules in heterogeneous catalysis and gas sensors. However, a limited understanding of interface chemistry and the involved mechanism impedes the development of a rational design of oxide interfaces for light‐activated gas sensing. Herein, the TiOx‐assisted photosensitization of In2O3 toward NO2 sensing is investigated as a case study to elucidate the detailed mechanism of light‐activated surface chemistry at the metal/gas interface. The resultant heterogeneous oxides exhibit outstanding NO2 sensing performance under light irradiation thanks to abundant photoexcited electrons and holes that serve as adsorption and desorption sites, respectively, to accelerate both surface reactions. Furthermore, the facile transfer of electrons and holes across the TiOx‐In2O3 interface contributes to improving the reversibility of sensing kinetics. Through this study, the mechanistic understanding is established of how the surface chemistry of metal oxide surfaces can be tuned by light activation providing an effective route to the design fabrication of high‐performance gas sensors. [ABSTRACT FROM AUTHOR]