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Metal‐Organic Frameworks (MOFs) have been used to catalyze the conversion of CO2 to cyclic carbonates through cycloaddition reaction. A series of MOFs composites based on Cu‐BTC (H3BTC, 1,3,5‐Benzenetricarboxylic acid) were screened out by adjusting the ligands and loaded materials. Among them, Cu‐BTC@ZnFe2O4 achieved good yields in this reaction, and after several catalytic cycles, the yield also remained above 90 %. The larger the steric hindrance of epoxides used, the lower the yields of cycloaddition reaction. In addition, computational chemistry was used to explain this catalytic process. After adding the catalyst, the energy barrier of the initial step of the reaction was effectively reduced. [ABSTRACT FROM AUTHOR]