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Herein, we report a highly controlled, solvent\u2010free, single\u2010precursor strategy utilizing 2,6\u2010diaminonaphthalene to synthesize ultrabright, highly uniform green\u2010emissive CDs (DAN\u2010CDs). Through comprehensive thermal analyses and kinetic modeling, we elucidate a spatiotemporally resolved, dual\u2010pathway formation mechanism: a nitrogen\u2010doped core initially assembles within an oxygen\u2010shielding autogenic precursor melt, followed by controlled, oxygen\u2010mediated surface passivation as the melt barrier attenuates. This self\u2010limiting oxidative capping thoroughly suppresses non\u2010radiative structural defects. Photophysical analyses uncover an efficient intra\u2010particle energy funneling process from the light\u2010harvesting core to these surface traps, yielding excitation\u2010independent green emission with a narrow bandwidth (&lt; 60\u00a0nm) and a near\u2010unity photoluminescence quantum yield of 91%. When integrated into self\u2010emissive light\u2010emitting diodes (LEDs), the devices deliver pure green electroluminescence. Notably, the peak external quantum efficiency (EQE) of 2.2% achieved herein through the solvent\u2010free approach stands as the highest value reported to date among LEDs based on green\u2010emissive CDs synthesized via thermal carbonization. These results conclusively underscore the strong potential of rationally designed DAN\u2010CDs as highly efficient, environmentally benign, and heavy\u2010metal\u2010free emitters for next\u2010generation optoelectronics and display applications.<\/jats:p>","DOI":"10.1002\/advs.77885","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T18:00:31Z","timestamp":1790532031000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Solvent\u2010Free Synthesis of Ultrabright Carbon Dots With Near\u2010Unity Quantum Yield for High\u2010Performance Light\u2010Emitting Diodes"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-0139-961X","authenticated-orcid":false,"given":"Hyeonjin","family":"Park","sequence":"first","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-2884-1864","authenticated-orcid":false,"given":"Su Hwan","family":"Lee","sequence":"additional","affiliation":[{"name":"Department of Energy Engineering Hanyang University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-0161-6859","authenticated-orcid":false,"given":"Sejeong","family":"Seo","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-0836-2506","authenticated-orcid":false,"given":"Soye","family":"Park","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Soo min","family":"Ji","sequence":"additional","affiliation":[{"name":"Department of Battery Engineering Hanyang University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-2387-160X","authenticated-orcid":false,"given":"Hyunda","family":"Jo","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-3879-1036","authenticated-orcid":false,"given":"Sehyeon","family":"Park","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1810-6885","authenticated-orcid":false,"given":"Young\u2010Hoon","family":"Kim","sequence":"additional","affiliation":[{"name":"Department of Energy Engineering Hanyang University  Seoul Republic of Korea"},{"name":"Department of Battery Engineering Hanyang University  Seoul Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9362-7686","authenticated-orcid":false,"given":"Woosung","family":"Kwon","sequence":"additional","affiliation":[{"name":"Department of Chemical and Biological Engineering Sookmyung Women's University  Seoul Republic of Korea"},{"name":"Institute of Advanced Materials and Systems Sookmyung Women's University  Seoul Republic of Korea"},{"name":"Trion Co. 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