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Here, we demonstrate an ion-regulated dynamic confinement strategy within 1.5 nm 2D silicate galleries that overcomes this classical trade-off. We reveal that intrinsic sodium ions (Na+) function as dynamic \u201cmolecular clutches\u201d at the organic\u2013inorganic interface. Rather than acting as static spacers, these confined ions reshape the interfacial thermodynamic landscape, enabling rapid coordination reconfiguration under extreme mechanical stimuli. This multiscale transformation dissipates extreme impact energy via intramolecular flattening and the formation of a highly ordered sacrificial phase, achieving a theoretically computed local ordering of \u223c85% within the nanoconfined galleries under an extreme 90% compressive strain, while maintaining an experimental bulk ordering of \u223c19% at the same macroscopic deformation limit (characterized by a highly aligned transition-state orientation angle of 18.3\u00b0). Consequently, this supramolecular network sustains a compressive stress of 380 MPa at a 95% strain without catastrophic fragmentation, delivering a volumetric energy dissipation of 68.68 J cm\u20133 with an energy conversion efficiency of \u223c87.8%. This study highlights the potential of nanoconfined ion-mediated mechanochemistry as a versatile design strategy for next-generation materials capable of extreme energy dissipation.<\/jats:p>","DOI":"10.1021\/jacs.6c09192","type":"journal-article","created":{"date-parts":[[2026,8,13]],"date-time":"2026-08-13T18:02:12Z","timestamp":1786644132000},"page":"35835-35847","source":"Crossref","is-referenced-by-count":0,"title":["Mechanochemically\nTriggered Conformational Reordering\nvia Ion-Regulated Molecular Clutches in Nanoconfined Networks"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-3640-9657","authenticated-orcid":true,"given":"Jiaxuan","family":"Liu","sequence":"first","affiliation":[{"name":"Guangzhou Medical University , , ,","place":["Guangzhou, P.R. China, 511436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Yuan","sequence":"additional","affiliation":[{"name":"Guangzhou Medical University , , ,","place":["Guangzhou, P.R. China, 511436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yichao","family":"Guo","sequence":"additional","affiliation":[{"name":"Guangzhou Medical University , , ,","place":["Guangzhou, P.R. China, 511436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenchen","family":"Wei","sequence":"additional","affiliation":[{"name":"Guangzhou Medical University , , ,","place":["Guangzhou, P.R. China, 511436"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8045-3856","authenticated-orcid":true,"given":"Jundong","family":"Shao","sequence":"additional","affiliation":[{"name":"Guangzhou Medical University , , ,","place":["Guangzhou, P.R. China, 511436"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,13]]},"reference":[{"key":"2026090104513204000_cit1","doi-asserted-by":"publisher","first-page":"2420717","DOI":"10.1002\/adfm.202420717","article-title":"Double-Crosslinked Organic\u2013Inorganic\nHybrid Polyimide Aerogel Composites with Ultra-Robust Toughness for\nFoldable Mechanical-Thermal-Coupled Protection","volume":"35","author":"Chen","year":"2025","journal-title":"Adv. Funct. Mater."},{"key":"2026090104513204000_cit2","doi-asserted-by":"publisher","first-page":"106684","DOI":"10.1016\/j.porgcoat.2021.106684","article-title":"State of the art and current trends\non layered inorganic-polymer nanocomposite coatings for anticorrosion\nand multi-functional applications","volume":"163","author":"Teijido","year":"2022","journal-title":"Prog. 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