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Oxidation of styrene is a key reaction in the synthesis of pharmaceuticals and fine chemicals, and therefore oxidizing styrene with selective, efficient, and recyclable heterogeneous catalysts is significant from an environmental and economic standpoint. In this study, we report the transition Cr-based metal-organic framework [NH 2 -MIL-101(Cr)] as a heterogeneous photocatalyst, which efficiently promotes styrene epoxidation using H 2 O 2 as a green oxidant, achieving high conversion efficiency (98%) and excellent selectivity (82%) under ambient conditions. Radical detection and quenching experiments reveal that the superoxide radical anion (O 2 ˙ - ) acts as an active oxygen species, selectively promoting the oxidation of styrene to its oxidized form. This work provides insight into the development of a sustainable and cost-effective method for producing styrene oxide.