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Noncovalent systems are adaptive and allow facile processing and recycling. Can they be at the same time robust? How can one rationally design such systems? Can they compete with high-performance covalent materials? The recent literature reveals that noncovalent systems can be robust yet adaptive, self-healing, and recyclable, featuring complex nanoscale structures and unique functions. We review such systems, focusing on the rational design of strong noncovalent interactions, kinetically controlled pathway-dependent processes, complexity, and function. The overview of the recent examples points at the emergent field of noncovalent nanomaterials that can represent a versatile, multifunctional, and environmentally friendly alternative to conventional covalent systems.