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Hierarchical self‐assembly is one of the most effective approaches to fabricate nature‐inspired materials with subtle nanostructures. We report a distinct hierarchical self‐assembly process of molecular double brushes (MDBs) with each graft site carrying a poly(azobenzene‐acrylate) (PAzo) chain and a poly(ethylene oxide) (PEO) chain. Asymmetric tapered worm (ATW) nanostructures with chain‐end reactivity...