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Conventional hydrothermal routes demand high temperature and pressure, while ambient\u2010pressure alternatives rely on strong acids and yield limited quantum yields without programmable surface control. This work reports a catechol\u2010assisted ambient\u2010pressure strategy that achieves hundred\u2010gram\u2010scale preparation of R\u2010CDs by simple heating at \u223c90\u00b0C. Catechol acts as a co\u2010polymerization mediator, participating in formation of carbon dots while its dual hydrogen\u2010bonding network suppresses functional\u2010group detachment, stabilizes radical intermediates, and lowers the steric barrier for cyclization. This mechanism enables programmable tuning of hydrophilicity\/hydrophobicity and emission wavelength by varying the precursor substituents. The hydrophobic carbon dots exhibit a solid\u2010state quantum yield of 45.26% (encapsulated in polyvinylpyrrolidone), the highest reported, and enable white light\u2010emitting diodes (WLED) with a color rendering index (CRI) of 94. The hydrophilic carbon dots (quantum yield 37.86%) are directly applied to deep\u2010tissue in vivo imaging without surface modification. This work provides a versatile molecular engineering platform for sustainable synthesis of functional aromatic carbon nanomaterials.<\/jats:p>","DOI":"10.1002\/anie.4229572","type":"journal-article","created":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T03:05:18Z","timestamp":1791601518000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Catechol as a Co\u2010Polymerization Mediator for Programmable Surface Chemistry Structure Synthesis of Carbon Dots"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-2488-6824","authenticated-orcid":false,"given":"Xiangyong","family":"Meng","sequence":"first","affiliation":[{"name":"College of Materials Science and Engineering College of Textiles and Clothes College of Physics School of Stomatology State Key Laboratory of Bio\u2010Fibers and Eco\u2010Textiles Qingdao University  Qingdao P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fumin","family":"Zheng","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering College of Textiles and Clothes College of Physics School of Stomatology State Key Laboratory of Bio\u2010Fibers and Eco\u2010Textiles Qingdao University  Qingdao P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1057-9522","authenticated-orcid":false,"given":"Haiguang","family":"Zhao","sequence":"additional","affiliation":[{"name":"College of Materials Science and Engineering College of Textiles and Clothes College of Physics School of Stomatology State Key Laboratory of Bio\u2010Fibers and Eco\u2010Textiles Qingdao University  Qingdao P.R. 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