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The development of thin layer on hollow-fiber substrate has drawn great attention in the gas-separation process. In this work, polydimethysiloxane (PDMS)/polyetherimide (PEI) hollow-fiber membranes were prepared by using the dip-coating method. The prepared membranes were characterized by Scanning Electron Microscope (SEM), energy-dispersive X-ray spectroscopy (EDX), and gas permeance measurements. The concentration of PDMS solution and coating time revealed an important influence on the gas permeance and the thickness of the PDMS layer. It was confirmed from the SEM and EDX results that the PDMS layer’s thickness and the atomic content of silicon in the selective layer increased with the growth in coating time and the concentration of PDMS solution. The composite hollow-fiber membrane prepared from 15 wt% PDMS solution at 10 min coating time showed the best gas-separation performance with CO₂ permeance of 51 GPU and CO₂/N₂ ideal selectivity of 21.