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Global warming and climate change concerns are triggering worldwide interest for sustainable transformation of CO2 into useful chemicals. Here, a new and efficient multifunctional catalytic system for the cycloaddition of carbon dioxide with epoxides to synthesize cyclic carbonates under mild and solvent-free reaction conditions has been developed. The catalytic tests revealed that [P-12,P-4,P-4,P-4]Br/MIL-53(Cr) (MIL: Materials of Institut Lavoisier) was the best and powerful catalytic system in the cycloaddition with excellent yields (96-99%) under solvent-free condition and 100 degrees C, 1.0MPa for 2-3h. The synergistic effect of anion and cation of ionic liquid [P-12,P-4,P-4,P-4]Br as well as the chromium site of cocatalyst MIL-53(Cr) contributed to the excellent catalytic activity. The present catalytic system has several unique features such as simple operation, good to excellent yields, high catalytic activity, environmentally benign and safe. This study provides a sustainable and efficient synergistic strategy for chemical carbon dioxide fixation via the combination of ionic liquids and metal-organic frameworks.