CeO2 with different morphologies (nanoparticles/NP, nanorods/NR, nanocubes/NC, nano‐octahedra/NO) are synthesized and decorated on BiOI nanoplates substrates to form CeO2@BiOI composites, which are used for aqueous Cr(VI) degradation. The intersurface states between BiOI and diverse CeO2 nanoparticles exhibit distinct behaviors when checked by XPS and photoluminescence intensity. The Cr(VI) degradation results show that the synthesized CeO2@BiOI nanocomposites possess higher photocatalytic activity than pure CeO2 or BiOI, and the CeO2‐NP@BiOI nanocomposite (molar ratio of CeO2: BiOI = 1:2) is the best one among them, with which the Cr(VI) is degraded up to 95.0% after 30 min irradiation using it as the photocatalyst. The superior catalytic performance of CeO2‐NP@BiOI can be attributed to a higher Ce3+ ratio of CeO2‐NP, a larger specific surface area, relatively low OH/CO32− content on the composite surface, and especially the good interaction between the CeO2 (111) facet and the BiOI surface.
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