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The efficient separation of gases has industrial, economic, and environmental importance. Here, we report the improvement in gas separation performance of a polyimide-based matrix (Matrimid^®5218) filled with a Cu-based metal organic framework [MOF, Cu₃(BTC)₂] with two different ionic liquids (ILs) confined within the pores. The chosen ILs are commonly used in gas solubilization, 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM][BF₄]) and 1-Ethyl-3-methylimidazolium trifluoromethanesulfonate ([EMIM][OTf]), and the incorporation of the [EMIM][BF₄]@Cu-BTC and [EMIM][OTf]@Cu-BTC composites in Matrimid^®5218 proved to be an efficient strategy to improve the permeability and selectivity toward CO₂/N₂ and CO₂/CH₄ mixtures.