Membranes offer improved energy efficiency in separations processes such as CO2 capture from combustion point sources, natural gas sweetening, syngas processing and air separation. To this end, a number of advanced polymer, inorganic and hybrid materials have been developed in recent years. Several distinct material classes have emerged, each with its respective set of benefits and limitations. Specifically, polyimides, ionic liquids (ILs), polymers of intrinsic microporosity (PIMs), metal-organic frameworks (MOFs) and thermally rearranged (TR) polymers are at the forefront of advanced membrane materials. We have identified a versatile approach which incorporates the benefits of these structurally diverse materials into a single platform through the synthesis of hybrid polyimide-ionene architectures, or “aromatic ionic polyimides”. This presentation will detail the design of these materials and their performances as gas separation membranes using both experimental data and computational studies.