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However, customizing their afterglow emission remains a major challenge. Here, we propose a machine learning\u2010guided strategy for tailored synthesis of single room\u2010temperature phosphorescent CDs from complex precursors, allowing programmable control over phosphorescence emission wavelengths and lifetimes. These single CDs are efficiently prepared via microwave\u2010assisted heating by tuning precursor compositions and subsequent separation from the in situ confined domains. Experimental findings reveal that the nitrogen dopant from urea governs the energy\u2010level structure of CDs, while a self\u2010protected superficial amorphous rigid network formed by sodium hydroxide and urea can stabilize triplet excitons, collectively enabling precise regulation of phosphorescence emission. Leveraging machine learning to model these multivariate relationships, we achieve on\u2010demand phosphorescent CDs with tunable emission wavelengths from 429 to 586\u00a0nm and lifetimes spanning from 3 to 2500\u00a0ms. The tailored CDs exhibited excellent performances in time\u2010resolved multilevel encryption, mechanically flexible afterglow devices, and white LEDs with persistent afterglow and outstanding operational stability (T\n                    <jats:sub>95<\/jats:sub>\n                    @10000\u00a0cd m\n                    <jats:sup>\u22122<\/jats:sup>\n                    = 22.76 h). This work establishes a rational pathway for designing intelligent luminescent materials and unlocks their potentials in secure labeling, anti\u2010counterfeiting technologies, and next\u2010generation optoelectronics.\n                  <\/jats:p>","DOI":"10.1002\/smll.74301","type":"journal-article","created":{"date-parts":[[2026,6,23]],"date-time":"2026-06-23T17:34:04Z","timestamp":1782236044000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Machine Learning\u2010Guided Tailored Synthesis of Single Room\u2010Temperature Phosphorescent Carbon Dots"],"prefix":"10.1002","volume":"22","author":[{"given":"Yu\u2010Qian","family":"Lin","sequence":"first","affiliation":[{"name":"School of Physical Science and Technology Guangxi University  Nanning China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng\u2010Long","family":"Shen","sequence":"additional","affiliation":[{"name":"Henan Key Laboratory of Diamond Material and Devices Key Laboratory of Material Physics School of Physics and Laboratory of Zhongyuan Light Ministry of Education Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi\u2010Ge","family":"Lv","sequence":"additional","affiliation":[{"name":"Henan Key Laboratory of Diamond Material and Devices Key Laboratory of Material Physics School of Physics and Laboratory of Zhongyuan Light Ministry of Education Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao\u2010Nan","family":"Lai","sequence":"additional","affiliation":[{"name":"Henan Key Laboratory of Diamond Material and Devices Key Laboratory of Material Physics School of Physics and Laboratory of Zhongyuan Light Ministry of Education Zhengzhou University  Zhengzhou 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Education Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chun\u2010Sheng","family":"Xie","sequence":"additional","affiliation":[{"name":"School of Physical Science and Technology Guangxi University  Nanning China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sheng","family":"Cao","sequence":"additional","affiliation":[{"name":"School of Physical Science and Technology Guangxi University  Nanning China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qing","family":"Lou","sequence":"additional","affiliation":[{"name":"Henan Key Laboratory of Diamond Material and Devices Key Laboratory of Material Physics School of Physics and Laboratory of Zhongyuan Light Ministry of Education Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chong\u2010Xin","family":"Shan","sequence":"additional","affiliation":[{"name":"Henan Key Laboratory of Diamond Material 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