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Here, we present a supramolecular engineering approach for precise drug delivery and real\u2010time monitoring of platinum(II) agents during therapy. Specifically, near\u2010infrared (NIR)\u2010emissive platinum(II) complex\u2010based polymeric nanomicelles were fabricated via electrostatic assembly, which enable sustained release of cytotoxic platinum(II) agents at tumor sites with deep tumor penetration. Crucially, the released platinum(II) monomer exhibits bright green phosphorescence upon binding to DNA. This generates a complementary dual\u2010emissive system: NIR emission from the platinum(II) oligomers allows in vivo imaging of biodistribution, while visible green emission from DNA\u2010bound monomers enables real\u2010time monitoring of drug\u2010target interaction dynamics. Photophysical mechanistic studies reveal that monomeric platinum(II) complexes undergo fast nonradiative decay governed by intramolecular vibronic wavefunction overlap. For oligomeric species, extended intermetallic interactions weaken exciton\u2010vibration coupling and correspondingly reduce vibronic overlap between electronic states, thereby suppressing nonradiative dissipation and enhancing luminescence efficiency. The nanomicelles exhibit remarkable tumor\u2010targeting selectivity and prolonged retention in tumor tissues, achieving significant tumor regression in vivo through synergistic chemo\u2010photodynamic therapy, with a 92.2% reduction in tumor volume. This supramolecular strategy overcomes key challenges in platinum\u2010based therapeutics and provides an integrated paradigm with strong potential for precision oncology.<\/jats:p>","DOI":"10.1002\/smll.75423","type":"journal-article","created":{"date-parts":[[2026,8,24]],"date-time":"2026-08-24T06:21:53Z","timestamp":1787552513000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Theranostic Platinum(II) Supramolecular Assembly: Differential Excited\u2010State Dynamics Enabling Synergistic Chemo\u2010Photodynamic Therapy With Real\u2010Time Tracking"],"prefix":"10.1002","author":[{"given":"Jian","family":"Zhao","sequence":"first","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory For Biomedical Research, School of Chemistry and Chemical Engineering Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yancheng","family":"Bai","sequence":"additional","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory For Biomedical Research, School of Chemistry and Chemical Engineering Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qin","family":"Ban","sequence":"additional","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory For Biomedical Research, School of Chemistry and Chemical Engineering Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunxia","family":"Song","sequence":"additional","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory For Biomedical Research, School of Chemistry and Chemical Engineering Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junqi","family":"Huang","sequence":"additional","affiliation":[{"name":"School of Pharmacy China Pharmaceutical University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengmin","family":"Shi","sequence":"additional","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory For Biomedical Research, School of Chemistry and Chemical Engineering Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4974-9496","authenticated-orcid":false,"given":"Gang","family":"Xu","sequence":"additional","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory For Biomedical Research, School of Chemistry and Chemical Engineering Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4945-2417","authenticated-orcid":false,"given":"Lei","family":"Fang","sequence":"additional","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory For Biomedical Research, School of Chemistry and Chemical Engineering Southeast University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,8,23]]},"reference":[{"key":"e_1_2_9_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.5b00597"},{"key":"e_1_2_9_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41568\u2010020\u201000308\u2010y"},{"key":"e_1_2_9_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jconrel.2025.02.006"},{"key":"e_1_2_9_5_1","doi-asserted-by":"crossref","DOI":"10.1016\/j.ccr.2024.215676","article-title":"Recent Advances in Nanocarriers for Clinical Platinum(II) Anticancer Drugs","volume":"505","author":"Zhang J. 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