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Spherical micelles assemble upon exposure to green light (530 nm), capture hydrophobic cargo, and then release said cargo upon disassembly with 365 nm irradiation; this cycle can be repeated at least 10 times without fatigue. One-step postsynthetic modification of the DNA backbone enables this technology, achieving the location-specific, multivalent attachment of light-responsive units without compromising the recognition of complementary DNA. 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