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Harnessing the structure\u2010property\u2010function relationships represents a practical strategy toward smart and effective nanomedicine. A structurally novel hydrogen\u2010bonded (H\u2010bonded) supramolecular nanoformulation generated by orthogonal self\u2010sorting assembly of chemo\u2010prodrug (FPtF) and phototherapeutics (BPeB) is here reported, to reach an autonomous nanomedicine with improved anti\u2010tumor efficacy by combining chemo\/phototherapy (CT\/PT). The high\u2010fidelity of H\u2010bonding modularity from privileged heterocomplementary diaminopyridine\/5\u2010fluorouracil (DAP\/FU) and Hamilton wedge\/barbiturate (HW\/Ba) pairs, respectively enable the precise spatial control of binding interactions toward FPtF and BPeB, in turn allowing the self\u2010sorting process and specific \u201cmix\u2010and\u2010match\u201d capability. To directly stimulate phototherapy from BPeB via near\u2010infrared (NIR) light, spectral matched upconversion nanoparticles (UCNPs, \u03b2\u2010NaYF\n                    <jats:sub>4<\/jats:sub>\n                    :Yb,Er) are encapsulated simultaneously. As a result, supramolecular polymeric nanomicelles, i.e., F\/B\/U@PHDO, are readily fabricated. Moreover, distinct H\u2010bonding association constant (Ka) of DAP\/FU (\u224810\n                    <jats:sup>2<\/jats:sup>\n                    \u00a0M\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and HW\/Ba (\u224810\n                    <jats:sup>4\u20105<\/jats:sup>\n                    \u00a0M\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) pairs reflect different strengths and stabilities of H\u2010bonds, thus endowing the programmable H\u2010bonding dissociation, accompanied with the chemo\u2010prodrug release through pH\/thermal\u2010stimuli. Therapeutic regime with appreciated anti\u2010tumor outcomes is ultimately accomplished via combined CT\/PT. The privileged opportunities offered by self\u2010sorting design are anticipated to point to new paradigm toward precise nanomedicine for cancer therapy.\n                  <\/jats:p>","DOI":"10.1002\/adma.202502416","type":"journal-article","created":{"date-parts":[[2025,4,7]],"date-time":"2025-04-07T03:46:50Z","timestamp":1743997610000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["\u201cMix\u2010and\u2010Match\u201d: Self\u2010Sorting Assembly Governed Supramolecular Polymeric Nanomedicine for Boosting Combined Chemo\/Phototherapy"],"prefix":"10.1002","volume":"37","author":[{"given":"Yanggui","family":"Wu","sequence":"first","affiliation":[{"name":"Hubei Engineering Research Center for Biomaterials and Medical Protective Materials School of Chemistry and Chemical Engineering Huazhong University of Science and Technology  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ting","family":"Li","sequence":"additional","affiliation":[{"name":"Cosme Biotechnology Co., Ltd.  Wuhan 430\u00a0074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zeke","family":"Li","sequence":"additional","affiliation":[{"name":"Hubei Engineering Research Center for Biomaterials and Medical Protective Materials School of Chemistry and Chemical Engineering Huazhong University of Science and Technology  Wuhan 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fr\u00e9d\u00e9ric","family":"Lortie","sequence":"additional","affiliation":[{"name":"Universite Claude Bernard Lyon 1 INSA Lyon Universit\u00e9 Jean Monnet CNRS UMR 5223 Ing\u00e9nierie des Mat\u00e9riaux Polym\u00e8res  C\u00e9dex F\u201069621 France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Julien","family":"Bernard","sequence":"additional","affiliation":[{"name":"Universite Claude Bernard Lyon 1 INSA Lyon Universit\u00e9 Jean Monnet CNRS UMR 5223 Ing\u00e9nierie des Mat\u00e9riaux Polym\u00e8res  C\u00e9dex F\u201069621 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