The release of excessive carbon dioxide (CO2) into the atmosphere poses potential threats to the well-being of various species on Earth as it contributes to global working. Therefore, it is necessary to implement appropriate actions to moderate CO2 emissions. A hollow fiber membrane contactor is an emerging technology that combines the advantages of separation processes and chemical absorptions. This study investigates the efficacy of wet and falling film membrane contactors (FFMC) in enhancing CO2 absorption in a monoethanolamine (MEA) aqueous solution. By analyzing factors such as membrane surface area, gas flow rate, liquid inlet flow rates, gas–liquid contact time, and solvent loading, we examine the CO2 absorption process in both contactors. Our results reveal a clear advantage of FFMC, achieving an impressive 85% CO2 removal efficiency compared to 60% with wet membranes. We employ COMSOL Multiphysics 6.1 simulation software and finite element analysis to validate our findings, demonstrating a close agreement between predicted and experimental values, with an average relative error of approximately 4.3%. These findings highlight the significant promise of FFMC for applications in CO2 capture.