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Nevertheless, most NIR\u2010II fluorescent probes, especially cyanine, are highly susceptible to self\u2010quenching in the aggregated state, which severely limits their application in bioimaging. Here, the Br\u2010modified cyanine dye F<jats:sub>4<\/jats:sub>\u2010Br and the amphiphilic polypeptide poly(oligo[ethylene glycol]methacrylate)\u2010<jats:italic>b<\/jats:italic>\u2010poly(benzyl\u2010L\u2010aspartic acid) (POEGMA\u2010PBLA) are\u00a0synthesized. By modulating the self\u2010assembly of F<jats:sub>4<\/jats:sub>\u2010Br and POEGMA\u2010PBLA to effectively inhibit the H\u2010aggregation of F<jats:sub>4<\/jats:sub>\u2010Br in aqueous solutions, nanoprobe F<jats:sub>4<\/jats:sub>\u2010Br@P<jats:sub>17<\/jats:sub> with outstanding antiquenching capability is\u00a0developed. This prominent feature allows it to perform vascular microscopic imaging with high spatiotemporal resolution and assess hemodynamic characteristics. F<jats:sub>4<\/jats:sub>\u2010Br@P<jats:sub>17<\/jats:sub> nanoparticles (NPs) with good stability and satisfactory biocompatibility also enable high contrast brightness for NIR\u2010II FL imaging of tumors. Given the efficient enrichment at tumor sites and the promising photothermal conversion efficiency (43.5%), F<jats:sub>4<\/jats:sub>\u2010Br@P<jats:sub>17<\/jats:sub> NPs successfully conduct photothermal therapy and exhibit superior antitumor efficiency under 1064\u00a0nm laser irradiation. These remarkable performances reveal the tremendous possibility of F<jats:sub>4<\/jats:sub>\u2010Br@P<jats:sub>17<\/jats:sub> NPs for in vivo\u00a0microscopic imaging and FL imaging\u2010guided photothermal therapy in the NIR\u2010II region.<\/jats:p>","DOI":"10.1002\/adhm.202300541","type":"journal-article","created":{"date-parts":[[2023,4,29]],"date-time":"2023-04-29T04:14:41Z","timestamp":1682741681000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["Antiaggregation of NIR\u2010II Probe Regulated by Amphiphilic Polypeptide with High Contrast Brightness for Phototheranostics and Vascular Microscopic Imaging under 1064\u00a0nm Irradiation"],"prefix":"10.1002","volume":"12","author":[{"given":"Changchang","family":"Teng","sequence":"first","affiliation":[{"name":"Department of Hepatobiliary Surgery The First Affiliated Hospital of USTC Division of Life Sciences and Medicine University of Science and Technology of China  Jinzai road 96 Hefei Anhui 230026 P. 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