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Petroleum depletion and climate change have inspired research on bio-based polymers and CO2 capture. Tung-oil-based polyols were applied to partially replace polyether-type polyols from petroleum for sustainable polyurethane. Tung-oil-based polyurethane (TBPU), was prepared via a two-step polycondensation, that is, bulk prepolymerization and chain extension reaction. The graphene oxide (GO) was prepared via Hummer's method. Then, TBPU was composited with the GO at different ratios to form a TBPU/GO hybrid film. The GO/TBPU films were characterized by fourier transform infrared spectroscopy (FTIR), differential scanning calorimeter (DSC), thermal gravimetric analysis (TGA) and scanning electron microscope (SEM), followed by the measurement of mechanical properties and gas permeability. The results showed that the addition of tung-oil-based polyols enhanced the glass transition temperature and thermal stability of TBPU. The mechanical properties of the hybrid film were significantly improved, and the tensile strength and elongation at break were twice as high as those of the bulk TBPU film. When the GO content was higher than 2.0%, a brittle fracture appeared in the cross section of hybrid film. The increase of GO content in hybrid films improved the selectivity of CO2/N-2 separation. When the GO content was higher than 0.35%, the resulting GO agglomeration constrained the gas separation and permeation properties.