| Summary: | Single-walled carbon nanotube buckypapers (SWCNT-bps) coated with a metal–organic framework ZIF-8 layer were used as supports for the preparation of Pebax<sup>®</sup> 3533 TFC membranes by both phase inversion and spin coating techniques. Upon proper characterization of the materials by X-ray diffraction, IR spectroscopy, thermogravimetry and electron microscopy, the obtained membranes were tested in gas separation experiments with a 15:85 CO<sub>2</sub>/N<sub>2</sub> mixture. These experiments proved that the ZIF-8 layer prevented from the penetration of the polymer selective film into the SWCNT-bp support, giving rise to a highly permeable selective membrane. The optimum membrane was achieved by the spin-coating method, with better permeation results than that prepared by the phase inversion method, obtaining a CO<sub>2</sub> permeance of 566 GPU together with a CO<sub>2</sub>/N<sub>2</sub> selectivity of 20.9.
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