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Crystal facet engineering (CFE) has been widely employed to regulate the photoreactivity of crystalline materials, mostly concerning the surface atomic and electronic structures. However, surface defects ubiquitous in real catalysts have long been less recognized. An integrated examination of various influence factors is necessary for the elucidation of an accurate structure–function relationship. Herein, we carefully studied the heterogeneous photoreactivity of CeO₂ nanocrystals (NCs) with well-defined crystal facets in multiple processes, including photocatalytic oxidation of volatile organic compounds (VOCs), O₂ evolution, and ·OH generation. Variable reactivity priorities were found between different nanoshapes as well as samples of identical nanoshapes. With integrated examinations of the coexisting surface factors (i.e., atomic, electronic, and defect structures), surface defects were evidently proved to compete …