Polymer membranes are critical to sustainability applications, and in this work we focused on one key application, the efficient separation of gas mixtures. Despite their widespread use, important challenges remain in the use of polymer membranes in this context – i.e., finding membrane materials with selectively improved transport of the desired mixture component(s) while possessing enhanced strength and improved aging behavior relative to the best current benchmarks. The important separation figures of merit are the gas flux, which is proportional to the permeability, Pi = Di × Si (Di is the gas diffusivity and Si its solubility coefficient) and selectivity (i.e., gas purity,αij = Pi/Pj). The goal is to simultaneously maximize Pi and αij. Most research to date has empirically targeted the development of new glassy polymers with improved separation performance. These include thermally rearranged (TR) polymers and polymers of intrinsic microporosity (PIMs).