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Here, we report a metal\u2013organic material in which water instead acts as a structural co\u2010monomer driving the formation of supramolecular fibers. A zinc(II) bisphenoxyimine (\u201cSalphen\u201d) complex featuring convergent hydrogen\u2010bond acceptor sites assembles in bulk water into long, hollow nanofibers stabilized by confined structural water molecules. Single\u2010particle analysis and density functional theory reveal tubular architectures in which intercalated water bridges the metal centers and defines a hydrophilic inner channel. The fibers form hydrogels with thermomechanical response, chemically triggerable disassembly and enable selective chiral recognition of amino acids via water\u2010mediated molecular\u2013to\u2013supramolecular information transfer. In organic solvents, the water content can be used for control over supramolecular self\u2010assembly and hence gelation and liquefaction. Our findings establish structural water as a design element for creating adaptive, chiral, and dynamically reconfigurable metal\u2013organic materials, offering a new paradigm to unlock this sustainable building block in supramolecular materials design.<\/jats:p>","DOI":"10.1002\/adma.202519933","type":"journal-article","created":{"date-parts":[[2026,1,22]],"date-time":"2026-01-22T11:18:18Z","timestamp":1769080698000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Hydrogelation via Supramolecular Copolymerization of Structural Water within Adaptive Metal\u2013Organic Fibers"],"prefix":"10.1002","volume":"38","author":[{"given":"Merlin R.","family":"St\u00fchler","sequence":"first","affiliation":[{"name":"Makromolekulare Chemie Universit\u00e4t Bayreuth  Bayreuth Germany"},{"name":"Institut F\u00fcr Chemie und Biochemie Freie Universit\u00e4t Berlin  Berlin 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