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Herein, we construct host\u2010guest metal\u2010organic framework (MOF) cocrystals employing a calcium\u2010based naphthalenediimide (NDI) host and electron\u2010rich aromatic guests to investigate photoinduced charge transfer at well\u2010defined crystalline donor\u2010acceptor interfaces. Challenging the conventional view that a high concentration of radical anions is typically associated with high photothermal conversion efficiency, our study uses electron paramagnetic resonance, surface photovoltage spectroscopy, and femtosecond transient absorption microscopy to show that a more extended conjugated plane in the guest accelerates charge recombination (charge\u2010transfer state lifetime: 201 vs. 348\u00a0ps). This leads to a MOF cocrystal with a photothermal conversion efficiency twice that of its counterpart, despite the latter exhibiting significantly higher NDI radical concentration. Moreover, this MOF cocrystal displays good aqueous stability and retains a photothermal conversion efficiency of 65.6% in aqueous media, enabling efficient near\u2010infrared light\u2010driven photothermal polymerization in both organic and aqueous phases. Notably, this photopolymerization proceeds even under natural sunlight irradiation and across biological tissue barriers. This work provides a novel design principle for donor\u2010acceptor materials, in which promoting charge recombination can be strategically exploited to develop high\u2010performance photothermal materials for solar energy utilization.<\/jats:p>","DOI":"10.1002\/anie.6791821","type":"journal-article","created":{"date-parts":[[2026,9,14]],"date-time":"2026-09-14T07:24:29Z","timestamp":1789370669000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Accelerated Charge Recombination in MOF Cocrystals Enables Efficient NIR\u2010Driven Photothermal Polymerization"],"prefix":"10.1002","author":[{"given":"Zhi","family":"Huang","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering National Institute for Advanced Materials Nankai University  Tianjin People's Republic of China"},{"name":"Tianjin Key Laboratory of Biosensing and Molecular Recognition Research Center for Analytical Sciences 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