Synthetic membranes facilitate the selective separation of specific molecules from mixtures. For example, membranes enable the production of clean water and safe pharmaceuticals. Unfortunately, the industrial manufacturing process used to produce membranes relies on the use of toxic solvents. In contrast, biological membranes leverage components that self-assemble to create multi-scale and hierarchical barriers that maintain unprecedented selectivity, controlling what and when molecules enter and exit cells. This Designing Materials to Revolutionize and Engineer our Future (DMREF) project seeks to harness biology-like performance and the chemical versatility of synthetic polymers. This looks to be achieved by mixing lipids, which are the building blocks of biological membranes, with charged polymers that can be synthesized to exhibit specific chemistries or charge patterns. These mixtures will spontaneously form nanoscale, ordered structures, that can form the basis for high-precision membranes. A major challenge is to design both lipids and polymers, which can have countless variations of chemical and physical features, to yield membranes for a given application. This project aligns with DMREF and the Materials Genome Initiative by combining materials synthesis and characterization with multi-scale molecular simulation and machine learning as the experiments will inform new computational models, which will then be used to expedite materials discovery to design new membranes.