This MRSEC, led by Columbia University in partnership with City College of New York, Harvard University, Barnard College, and the University of the Virgin Islands, encompasses two IRGs around the theme of building higher dimensional materials from lower dimensional structures with unprecedented levels of control. Both IRGs are built around techniques pioneered by the team, and bring together researchers with diverse capabilities, strong accomplishments, and a record of collaboration. The unified center will enable formation of the interdisciplinary teams required to undertake the proposed research, support of shared experimental tools, implementation of a multi-faceted program of education and human resources development, and focused efforts to improve diversity. The MRSEC leverages the proximity of Columbia, CCNY, and Barnard for intercampus cooperation, and nearby K-12 schools for educational activities. Brookhaven National Laboratory, IBM, DuPont, and other partners provide research partnerships and educational opportunities. Synergy among the two IRG teams includes the common emphasis on materials assembly with precise control, and is enhanced by co-advising of MRSEC Fellows and common educational activities.