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Herein, a novel CdIn2S4/In2O3 heterojunction photocatalyst, aiming to enhance photocatalytic performance for pollutant degradation, is fabricated by a self‐assembly process at low temperature. Ternary CdIn2S4 nanoparticles are uniformly deposited on the In2O3 nanoflowers, forming a step‐scheme (S‐scheme) hybrid heterostructure. As a result, the light absorption efficiency and charge separation efficiency of CdIn2S4/In2O3 are greatly improved. Among these fabricated samples are activated by visible light, and the degradation efficiency of gaseous acetone is as great as 92.3% over 10% CdIn2S4/In2O3 within 3 h, which is the highest value observed. Furthermore, the key intermediate compounds are elucidated using in situ Fourier transform infrared (FTIR) spectra, which strongly validate the hypothesized light degradation mechanism over CdIn2S4/In2O3. Correspondingly, a potential photocatalytic mechanism over CdIn2S4/In2O3 S‐scheme heterojunction is explored and discussed.