Carbon Nanotubes (CNTs) were synergistically integrated to polysulfone (PSF) to develop a highly selective mixed-matrix membranes (MMMs) for CO2 separation purpose in a presence of a metal organic framework (MOFs). This study aims to integrate CNTs with metal organic frameworks into a MMM to separate CO2 efficiently. The results show that filled MMMs with about 5 wt % CNTs showed an optimum separation performance by providing a CO2/N2 selectivity of about 50. Increasing CNTs additives resulted in in lowering the selectivity.