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The Crystal Growth and Assembly Gordon Research Conference is dedicated to the knowledge and understanding of the fundamental atomic and nanoscale physics and chemistry that are central to the nucleation and growth of crystals, as well as the assembly of crystalline units into ordered structures. This well-established conference draws researchers from around the world in the fields of physics, chemistry, engineering, materials science, biology, and beyond. Historically, the conference has emphasized concepts rather than specific materials, technologies or growth methods. This focus has attracted scientists with a broad range of specializations, including semiconductor nanowires and quantum dots, metal nanocrystals, biomineralization, soft matter, assembly, in situ microscopy, and multi-scale theory and simulation, who find common inspiration in seeing how the general principles of crystal thermodynamics and growth kinetics are applicable to many fields. The 2021 Crystal Growth and Assembly GRC will continue the tradition of a highly interdisciplinary program, highlighting the most recent developments in the field. Featured topics will be Nanocrystals, Assembly, Nucleation, Non-Classical Crystal Growth, the Liquid-Solid Interface, Organic, Bio-Inspired, and Biogenic Crystals, Synthesis Science of Crystalline Materials for Applications, and Directing Growth and Assembly from the Bottom Up. A particular focus will be on the interplay between theory and experiment in developing a mechanistic understanding of crystallization and assembly spanning a broad range of materials.