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However, the development of efficient NIR\u2010UOP systems remains challenging. In this study, we propose a rational molecular design strategy to achieve visible\u2010light\u2010excited (\n                    <jats:italic>\u03bb<\/jats:italic>\n                    <jats:sub>ex<\/jats:sub>\n                    = 450\u00a0nm) NIR\u2010UOP via excited\u2010state conformational dynamics. The optimized molecule, py\u20102mNO\n                    <jats:sub>2<\/jats:sub>\n                    , exhibits NIR\u2010UOP emission at 635 and 700\u00a0nm, with a high phosphorescence intensity of 12\u00a0cd\/m\n                    <jats:sup>2<\/jats:sup>\n                    and a lifetime of 268\u00a0ms. Mechanistic studies reveal that the dynamic conformational charge transfer facilitates intersystem crossing (ISC). Meanwhile, the relatively flat excited\u2010state potential energy surface enables the molecule to adopt a planar conformation, thereby suppressing non\u2010radiative decay through intramolecular attractive interactions. Leveraging these properties, py\u20102mNO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010based nanoparticles were assembled using a polymethyl methacrylate (PMMA) isolation strategy. Consequently, high\u2010contrast phosphorescence imaging of hypoxic tumors with a signal\u2010to\u2010background ratio (SBR) of 39.47 (\n                    <jats:italic>\u03bb<\/jats:italic>\n                    <jats:sub>e<\/jats:sub>\n                    <jats:sub>x<\/jats:sub>\n                    = 365\u00a0nm) was achieved using this matrix\u2010isolated phosphorescent nano\u2010assembly, which could even be excited with a commercial mobile phone flashlight (SBR = 14.55). This work not only provides a rational design strategy for visible\u2010light\u2010excited NIR\u2010UOP systems but also establishes an efficient nano\u2010assembly approach for constructing NIR\u2010UOP nanoparticles suitable for in vivo imaging.\n                  <\/jats:p>","DOI":"10.1002\/anie.5778721","type":"journal-article","created":{"date-parts":[[2026,7,26]],"date-time":"2026-07-26T18:01:26Z","timestamp":1785088886000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Excited\u2010State Conformational Dynamics Enables Visible\u2010Light\u2010Activated Near\u2010Infrared Phosphorescent Nano\u2010Assemblies for Bioimaging"],"prefix":"10.1002","volume":"65","author":[{"given":"Junru","family":"Chen","sequence":"first","affiliation":[{"name":"Matter School of Materials and Energy Guangdong University of Technology  Guangzhou P. R. 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