AbstractHollow fibre carbon membranes (HFCMs) were fabricated from deacetylated cellulose acetate precursors based on a multi-dwell carbonization protocol. Membrane structure and morphology were characterized by scanning electronic microscope (SEM), and membrane separation performances for single gas and gas mixtures were tested by the in-house gas test setup. Simulations of CO2 capture by hollow fibre carbon membranes were conducted based on Aspen Hysys® integrated with ChemBrane. The characteristic diagrams and optimal configuration were obtained, and the process was optimized based on the necessary membrane area, energy demands for the compressor and cooler, recovery and purity of CO2, and capital cost.