CO2-philic copper zinc bimetallic imidazolate framework (CuZnIF) particles were synthesized and introduced into poly (ether block amide) (PEBA) matrix in the range of 0.1–10 wt.% to fabricate mixed matrix membranes (MMMs) with enhanced performance for CO2 separation. The effects of nanoparticle loading and feed pressure on the separation performance of the MMMs were investigated. The CuZnIF particles were characterized by FTIR, FESEM, XRD, BJH and BET tests. The nanocomposite membrane containing 0.5 wt.% of CuZnIF showed the best performance; CO2 permeability, CO2/N2 and CO2/CH4 selectivity of MMMs were improved about 47, 61 and 30%, respectively.