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The UV light‐induced generation of colloidal molecules with precisely controlled structures is reported by Zhihong Nie, Yutao Sang and co‐workers in their Research Article (e202313406). Photolabile copolymer ligands are used to control the self‐assembly of complementary copolymer‐capped binary nanoparticles A and B into clustered ABx or linear (AB)y structures on demand.