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By combining emissive chromophores, optimized electronic structures, and confined microenvironments, it provides an effective strategy for enhancing cathodic electrochemiluminescence (ECL). Here, we report a discrete Pt(II)\u2010Ru(II) heterometallacycle constructed by embedding a Ru(II) polypyridyl luminophore into a positively charged Pt(II)\u2010based metallacyclic scaffold. The assembly reorganizes the frontier electronic structure through orbital redistribution and enhanced delocalization while preserving the intrinsic Ru(II)\u2010centered emissive excited state, thereby enabling efficient coupling between electrochemical reduction and excited\u2010state formation. Consequently, the heterometallacycle exhibits dramatically enhanced cathodic ECL, demonstrating that supramolecular electronic reconfiguration can overcome the intrinsic limitations of molecular luminophores. The positively charged cavity further enables 1:1 host\u2013guest complexation with terephthalate dianions, and guest encapsulation modulates the local electronic environment to produce an additional ECL enhancement. Notably, the binding constant determined by ECL titration agrees well with that obtained from fluorescence titration, establishing ECL as a complementary signal transduction modality for probing host\u2013guest recognition. This work demonstrates that coordination\u2010driven self\u2010assembly enables the synergistic integration of emissive chromophores, electronic regulation, and guest\u2010responsive supramolecular microenvironments, providing new design principles for supramolecular cathodic ECL systems.<\/jats:p>","DOI":"10.1002\/anie.7715295","type":"journal-article","created":{"date-parts":[[2026,9,17]],"date-time":"2026-09-17T03:49:04Z","timestamp":1789616944000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Coordination\u2010Driven Pt(II)\u2010Ru(II) Heterometallacycles With Ultrastrong Cathodic Electrochemiluminescence and Guest\u2010Responsive Signal Amplification"],"prefix":"10.1002","volume":"65","author":[{"given":"Zeyu","family":"Yang","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering Key Lab of Fuel Cell Technology of Guangdong Province South China University of Technology  Guangzhou China"},{"name":"Department of Biomedical Engineering Key Laboratory of Biomaterials of Guangdong Higher Education Institutes Jinan University  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1275-5887","authenticated-orcid":false,"given":"Jianshan","family":"Ye","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Key Lab of Fuel Cell Technology of Guangdong Province South China University of Technology  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2204-0663","authenticated-orcid":false,"given":"Ying","family":"Ma","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Key Lab of Fuel Cell Technology of Guangdong Province South China University of Technology  Guangzhou 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