The increasing need for more efficient separation processes has motivated the development of polymer membranes that can provide fast and selective transport. In this work, cadmium‐based metal–organic framework (MOF) nanoparticles and a polyurethane–urea (PUU) elastomer were synthesized. New mixed‐matrix membranes (MMMs) were then fabricated from the nanoparticles and the PUU. SEM images verified that embedding the nanoparticles changes the morphology of the PUU and the nanoparticles disperse well in the PUU due to satisfactory compatibility of the polymer and nanoparticles. Fourier transform infrared spectroscopy and X‐ray diffraction analysis confirmed the dispersion of the nanoparticles in the soft segment of the PUU. With increased temperature, gas permeabilities of the MMMs improved but their sieving ability deteriorated. An MMM incorporating 2.5 wt % of the MOF showed a CO2 permeability of ~140 barrer and a CO2/N2 selectivity of ~30, which are 89 and 38% higher than those of the pristine membrane. Gas permeation tests showed that the higher CO2/N2 selectivity of the MMMs was due to improved solubility selectivity and the higher CO2 permeability was a result of improved CO2 diffusivity and solubility coefficients. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 137, 48704.