This presentation will detail our development of new polymer architectures which contain high free volume elements (e.g., 6-FDA, spirobisindane, Tröger's Base, etc.) which are covalently bond to ionic groups forming gas separation membranes which not only can absorb ionic liquids (ILs) into their structures, but also align/rearrange in the presence of ILs. This "bottom-up" approach allows for high degrees of membrane tunability and influence/control over polymer nanostructure and associated performance with respect to gas separations involving CO2, N2, CH4, H2 and other species.