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Self-assembly enables hierarchical organization and compartmentalization of matter previously observed only in natural materials. Simple chemical motifs can be used to fabricate structures with diverse range of architectures and properties. The design principles, originally found in nature, are being implemented in self-assembled materials. The examples include high mechanical strength of bones and nacre achieved through hierarchical organic–inorganic organization, and DNA nanotechnology enabled by complementary bonding of DNA molecules. Building materials with controlled architectures from the nanoscale to the macroscale will lead to a combination of properties that will have significant impacts on fields ranging from tissue regeneration to optoelectronics.