The Northwestern University Materials Research Science and Engineering Center (NU-MRSEC) advances world-class materials research, education, and outreach via active interdisciplinary collaborations within the Center and with external partners in academia, industry, national laboratories, and museums, both domestically and abroad. The intellectual merit of the NU-MRSEC resides primarily within its interdisciplinary research groups (IRGs) and seed-funded projects that explore the frontiers of materials research. IRG-1 entitled ?Bioprogrammable Materials via Cell-Free Synthetic Biology? develops soft composite materials that incorporate biological machinery in a cell-free platform, thus removing the nourishment and care demands of living tissue. In this manner, the functionality of living biological systems are achieved in an autonomous material with direct implications for sustainable agriculture, water treatment, smart clothing, and wound healing. IRG-2 entitled ?Orchestrated Iontronics via Dynamic Hybrid Ionic/Electronic Conductors? designs materials that concurrently conduct ions and electrons, behaving in a manner that mimics biological neurons. These hybrid ionic/electronic conductors thus enable brain-inspired computation that is accelerating advances in artificial intelligence, robotics, and bioelectronics. By incorporating these research advances into innovative pedagogy, the NU-MRSEC achieves broad impact through professional development of graduate students and postdocs, research experiences for undergraduates and teachers, and outreach to K-12 students and the general public. These activities are enhanced by partnerships with Argonne National Laboratory, Art Institute of Chicago, Chicago Museum of Science and Industry, Chicago Field Museum of Natural History, Chicago Public Schools, and Chicago City Colleges.