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Here we show that single\u2010atom C\u2010to\u2010N skeletal editing in hemicyanine dyes precisely regulates intramolecular charge distribution and intermolecular packing, thereby allowing efficient formation of bright NIR\u2010II J\u2010aggregates. Systematic acceptor engineering reveals clear structure\u2010assembly\u2010property relationships governing J\u2010aggregate formation and fluorescence brightness. The optimized dye\n                    <jats:bold>HZOE9<\/jats:bold>\n                    forms stable J\u2010aggregates with emission beyond 1000\u00a0nm and a quantum yield surpassing most reported cyanine\u2010based NIR\u2010II fluorophores. Mechanistic studies further elucidate that phenolic hydroxyl modification can tune J\u2010aggregation and NIR\u2010II emission, highlighting its key role in modulating supramolecular excitonic coupling. Encapsulation into biocompatible nanoparticles enables high\u2010resolution lymphatic imaging, real\u2010time metastasis visualization, fluorescence\u2010guided surgery, and therapeutic monitoring in vivo. This work establishes a single\u2010atom skeletal editing strategy for developing hemicyanine\u2010based NIR\u2010II fluorophores and provides a conceptual framework for the future development of activatable NIR\u2010II fluorophores via controllable supramolecular assembly.\n                  <\/jats:p>","DOI":"10.1002\/anie.5207784","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T14:32:18Z","timestamp":1785940338000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Single\u2010Atom C\u2010to\u2010N Editing Unlocks Bright NIR\u2010II J\u2010Aggregates for Imaging Lymphatic Metastasis"],"prefix":"10.1002","volume":"65","author":[{"given":"Xing","family":"Wei","sequence":"first","affiliation":[{"name":"MOE Key Laboratory for Biomedical Photonics Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology  Wuhan 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