Membrane-based separations have revolutionized some industries (e.g., seawater desalination) and have the potential to drive numerous applications towards more energy efficient and sustainable processes. In chemical separations, which are typically highly energy intensive and account for greater than 5% of the annual primary energy consumption in the U.S., membrane-based approaches have significant potential to reduce both energy utilization and capital cost. However, membranes for the separation of mixed solvents, while practically important, are technically challenging as differentiating between the transport of small molecules that have subtle differences in properties is required. The rational design of the next generation of membranes for such separations is a significant challenge, given the vast chemical and design space, but could be realized by Materials Genome Initiative (MGI)-inspired screening. That is, the MGI-style of this effort could alter the current, long-standing membrane development paradigm. In this work, functionality- and performance-driven screening, with close coupling between simulations and experiment, will result in the design and fabrication of high-performance membranes tailored for targeted separations. Specifically, the dehydration of polar solvents by pervaporation will be targeted as an overarching initial target. This is because the discovery and deployment of effective new materials will eliminate the need for high-cost and high-energy separations and enable effective solvent reuse for sustainable manufacturing.