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Rapid Commun."],"published-print":{"date-parts":[[2026,9]]},"abstract":"<jats:title>ABSTRACT<\/jats:title>\n                  <jats:p>\n                    Poly (vinyl alcohol) (PVA), a representative biodegradable and water\u2010soluble polymer, suffers from high crystallinity, a strength\u2011toughness trade\u2011off, and poor thermal stability arising from strong interchain hydrogen bonding. Conventional modification strategies fail to simultaneously achieve synergistic enhancement of strength\u2010toughness and functionalization, severely restricting its engineering applications. Herein, inspired by the robust yet dynamic nature of cation\u2010\u03c0 interactions, we present a universal design strategy for high\u2010performance water\u2010soluble polymers based on indole\u2010Mg\n                    <jats:sup>2+<\/jats:sup>\n                    cation\u2010\u03c0 dynamic cross\u2010linking. Molecular simulations and spectroscopic characterization demonstrate that Mg\n                    <jats:sup>2+<\/jats:sup>\n                    forms strong cation\u2010\u03c0 interactions with indole moieties, exhibiting a binding energy of \u2212113\u00a0kJ\u00a0mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Mechanical testing reveals that the optimally formulated PVAI\u2010\n                    <jats:sub>7.5%<\/jats:sub>\n                    Mg\n                    <jats:sup>2+<\/jats:sup>\n                    film achieves a tensile strength of 51 MPa (a 130% increase from 22 MPa) and an elongation at break of 400% (enhanced from 320%), thereby realizing synchronous improvement of strength and toughness. Benefiting from the dynamic reversibility of cation\u2010\u03c0 interactions, the film exhibits autonomous scratch healing within 12 h at room temperature without external stimuli, while retaining excellent water solubility that enables multiple recovery and reprocessing cycles via solvent\u2010based methods without performance degradation. This study overcomes the dual bottlenecks of the strength\u2010toughness trade\u2010off and the performance\u2010functionalization incompatibility inherent to PVA modification, offering new avenues for the high\u2010performance and multifunctional design of water\u2010soluble polymers and providing experimental and theoretical insights into the application of cation\u2010\u03c0 interactions in polymeric materials.\n                  <\/jats:p>","DOI":"10.1002\/marc.70374","type":"journal-article","created":{"date-parts":[[2026,7,23]],"date-time":"2026-07-23T04:17:28Z","timestamp":1784780248000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Cation\u2010\u03c0 Dynamic Cross\u2010Linking Enabled High\u2010Performance PVA Films With Synchronous Strength\u2010Toughness Enhancement, Self\u2010Healing, and Recyclability"],"prefix":"10.1002","volume":"47","author":[{"given":"Yang","family":"Xu","sequence":"first","affiliation":[{"name":"State Key Laboratory for Environment\u2010Friendly Energy Materials &amp; Inertial Confinement Fusion Energy Materials Key Laboratory of Sichuan Province &amp; School of Materials and Chemistry Southwest University of Science and Technology  Mianyang People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinping","family":"Yu","sequence":"additional","affiliation":[{"name":"State Key Laboratory for Environment\u2010Friendly Energy Materials &amp; Inertial Confinement Fusion Energy Materials Key Laboratory of Sichuan Province &amp; School of Materials and Chemistry Southwest University of Science and Technology  Mianyang People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yiwen","family":"Lu","sequence":"additional","affiliation":[{"name":"State Key Laboratory for 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