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Herein, we unveil the ability of supramolecular polymers (SPs) formed by G\n                    <jats:sub>4<\/jats:sub>\n                    .Cu\n                    <jats:sup>+<\/jats:sup>\n                    to undergo heating\u2010induced unexpected aqueous phase transitions. For the first time, guided by Cu\n                    <jats:sup>+<\/jats:sup>\n                    , guanosine (G) formed a highly stable G\u2010quartet (G\n                    <jats:sub>4<\/jats:sub>\n                    .Cu\n                    <jats:sup>+<\/jats:sup>\n                    )\/G\u2010quadruplex as a non\u2010canonical DNA secondary structure with temperature tolerance, distinct from the well\u2010known G\n                    <jats:sub>4<\/jats:sub>\n                    .K\n                    <jats:sup>+<\/jats:sup>\n                    . The G\n                    <jats:sub>4<\/jats:sub>\n                    .Cu\n                    <jats:sup>+<\/jats:sup>\n                    self\u2010assembled in water through \u03c0\u2010\u03c0 stacking, metallophilic and hydrophobic interactions, forming thermally robust SPs. This enhanced stability is attributed to the stronger coordination of Cu\n                    <jats:sup>+<\/jats:sup>\n                    to four carbonyl oxygens of G\u2010quartet and the presence of Cu\n                    <jats:sup>+<\/jats:sup>\n                    \u2010\u2009\u2010\u2009\u2010Cu\n                    <jats:sup>+<\/jats:sup>\n                    attractive metallophilic interactions in Cu\n                    <jats:sup>+<\/jats:sup>\n                    \u2010induced G\u2010quadruplex, exhibiting a significantly higher interaction energy than K\n                    <jats:sup>+<\/jats:sup>\n                    as determined computationally. Remarkably, the aqueous SP solution exhibited heating\u2010induced phase transitions\u2014forming a hydrogel through dehydration\u2010driven crosslinking of SPs below cloud temperature (\n                    <jats:italic>T<\/jats:italic>\n                    <jats:sub>cp<\/jats:sub>\n                    ) and a hydrophobic collapse\u2010induced solid precipitate above\n                    <jats:italic>T<\/jats:italic>\n                    <jats:sub>cp<\/jats:sub>\n                    , showcasing a lower critical solution temperature (LCST) behavior. Notably, this LCST behavior of G\n                    <jats:sub>4<\/jats:sub>\n                    .Cu\n                    <jats:sup>+<\/jats:sup>\n                    SP originates from biomolecular functionality rather than commonly exploited thermo\u2010responsive oligoethylene glycols with supramolecular assemblies. Furthermore, exploiting the redox reversibility of Cu\n                    <jats:sup>+<\/jats:sup>\n                    \/Cu\n                    <jats:sup>2+<\/jats:sup>\n                    , we demonstrated control over the assembly and disassembly of G\u2010quartets\/G\u2010quadruplex and gelation reversibly.\n                  <\/jats:p>","DOI":"10.1002\/anie.202417508","type":"journal-article","created":{"date-parts":[[2025,1,20]],"date-time":"2025-01-20T11:19:42Z","timestamp":1737371982000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":20,"title":["Cu(I)\u2010Induced G\u2010Quartets: Robust Supramolecular Polymers Exhibiting Heating\u2010Induced Aqueous Phase Transitions Into Gel or Precipitate"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-3043-0557","authenticated-orcid":false,"given":"Nihar","family":"Sahu","sequence":"first","affiliation":[{"name":"Department of Chemistry 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