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Here we report a hierarchical composite strategy that embeds a one\u2010dimensional Zn(II) coordination polymer capable of topochemical [2+2] cycloaddition within a poly(vinyl alcohol) matrix and coats it with poly(\u03b5\u2010caprolactone), yielding mechanically robust, scalable, and water\u2010stable photomechanical films. The composites exhibit wavelength\u2010selective activation and expansion\u2010programmable deformation, enabling dual\u2010stage bending and radial expansion with actuation fidelity exceeding 98% over extended storage and radial strengths approaching those of load\u2010bearing polymeric systems. Comparative analysis across representative photoactuating materials identifies a distinct regime combining crystalline photochemical precision with macroscopic mechanical resilience. These results establish general design principles\u2014topochemical preorganization, hierarchical stress transfer, and protective coating\u2014for translating lattice\u2010confined photochemistry into durable, expansion\u2010programmable mechanical actuation, providing a foundation for next\u2010generation adaptive and deployable material systems.<\/jats:p>","DOI":"10.1002\/adma.74238","type":"journal-article","created":{"date-parts":[[2026,7,22]],"date-time":"2026-07-22T12:17:06Z","timestamp":1784722626000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Hierarchical Coordination Polymer\u2013Polymer Composites for Robust, Programmable Photomechanical Actuation"],"prefix":"10.1002","volume":"38","author":[{"given":"Shu\u2010Fen","family":"Zhang","sequence":"first","affiliation":[{"name":"College of Chemistry Chemical Engineering and Materials Science Soochow University  Suzhou P. R. 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