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Continued integration of technologies capable of achieving higher degrees of sustainability while meeting global material and energy demands is of singular importance in halting human-caused climate change. Gas separation membranes composed of metal–organic frameworks (MOFs) are considered promising candidates for such integration; owing to their modular, scalable nature and high degree of tunability they are seen essential to maintain separation functionality. However, prior to sustainable implementation, both an evaluation of MOF characteristics and an intensive examination of MOF–gas molecule interactions are necessary to fully understand the fundamental separation criteria as well as to define suitable ranges of gas separation conditions. Herein, we present our findings on the greenhouse gas separation capabilities of the hydrophilic, Al-based MIL-160 in the selective uptake of carbon dioxide (CO 2 ) from other relevant greenhouse gases, i.e. , methane (CH 4 ), sulfur dioxide (SO 2 ), nitrogen dioxide (NO 2 ), and nitric oxide (NO), including gravimetric solubility, permeability, and diffusivity calculations. We found that a MIL-160 membrane has excellent applicability in the separation of gases of varying electronegativities, with a diffusivity selectivity of 72.0, 9.53, and 13.8 for CH 4 , NO 2 , and NO, respectively, relative to CO 2 . Further, we demonstrate that the selectivity at which gas molecules diffuse through the MIL-160 membrane varies strongly with the simulation pressure, suggesting that such membrane system is potentially an ideal candidate for the development of pressure-swing adsorption processes that achieve gas separations efficiently while mitigating the emission of greenhouse gases.