AbstractDifferent top layer fabrication methods (amine‐first, acid‐first, spin coating), organic phase solvents (hexane, heptane, mixed hexane/heptane), acid acceptors (triethylamine, sodium carbonate, sodium hydroxide), and surfactant sodium dodecyl sulfate concentrations (0, 0.05, and 0.1 wt%) were utilized to fabricate thin film composite polyamide membranes for CO2/N2 separation. The results, according to an L9 orthogonal array of Taguchi approach, showed that employing acid‐first method increases both CO2 permeance and CO2/N2 selectivity of the membranes at a feed gas pressure of 3 bars. On the other hand, sodium hydroxide, and triethylamine should be used, as acid acceptors, to maximize CO2 permeance and CO2/N2 selectivity, respectively. Moreover, the use of hexane solvent and 0 wt% surfactant led to maximum permeance, while, hexane solvent and 0.1 wt% surfactant were needed to reach the highest selectivity. The above level setting of synthesis parameters also resulted in the minimum sensitivity of the fabrication process to the noise factors effects. As shown by the analysis of variance, acid acceptor, and organic solvent types were the most influential parameters on CO2 permeance and CO2/N2 selectivity, respectively. The effects of fabrication method and surfactant concentration, as single factors, on permeation/selectivity responses were also investigated.