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Nanocrystals—nanometer-sized inorganic crystals containing hundreds to thousands of atoms—offer exciting opportunities in areas as varied as photonics, catalysis, biotechnology, and medicine. For example, nanocrystals enrich the display color palette in tablet computers and advanced TVs. Two reports in this issue, by Zherebetskyy et al. on page 1380 (1) and Boneschanscher et al. on page 1377 (2), investigate nanocrystal surfaces and show how these surfaces can be merged in a controllable fashion, allowing the assembly of novel material architectures.