Novel NaA zeolite/carbon nanocomposite thin films were successfully prepared on a porous α-Al 2 O 3 substrate by dip-coating method. The prepared films were characterized by XRD, SEM and single gas permeation tests. NaA zeolite/carbon nanocomposite thin films exhibited the ideal separation factor of CO 2 /N 2 of 6.04 with the carbon dioxide permeance of 3.39×10 −7 molPa −1 m −2 s −1 at room temperature and 100kPa, which was two orders of magnitude higher than that of pure carbon membrane reported by previous literature. The observed adsorption isotherms indicated that the incorporation of zeolite NaA crystal improved the CO 2 adsorption ability of carbon materials, and decreased its N 2 adsorption ability. The ideal permselectivity of CO 2 /N 2 of carbon/NaA composite films was 6.04, higher than the ideal adsorption selectivity, probably because the small molecule of CO 2 diffused faster than N 2 . From the SEM images, the thickness of nanocomposite films was 1–2μm, which was helpful to decrease the resistance and increase the flux of gas permeance.