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However, the discovery of new lipid scaffolds remains constrained by the limited availability of efficient synthetic platforms capable of generating structurally diverse libraries. Here, we report a photochemistry-based ionizable lipid library (PILL) platform that enables the rapid discovery of ionizable lipids for mRNA delivery. Using a visible-light-driven multicomponent reaction under 427 nm irradiation, 275 \u03b1-branched amine-containing ionizable lipids were generated in a one-pot process from amines, aldehydes, and boronic acids under mild conditions. This modular photochemical strategy enabled the rapid construction of a structurally diverse lipid library that was directly integrated with purification-free in vitro screening and subsequent in vivo validation. A18B8C14 was identified as a lead ionizable lipid candidate for mRNA delivery, and the optimized A18B8C14-LNP formulation exhibited substantially higher in vivo gene expression than the benchmark MC3-based LNP while maintaining a favorable safety profile. In addition, organ-specific delivery could be achieved by adjusting the A18B8C14-LNP formulation according to the selective organ targeting (SORT) strategy. Together, these results establish photochemistry as a practical platform for ionizable lipid discovery and provide a versatile framework for the development of next-generation LNP systems for nucleic acid therapeutics.<\/jats:p>","DOI":"10.1021\/jacs.6c13674","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T03:54:33Z","timestamp":1787370873000},"page":"42494-42507","source":"Crossref","is-referenced-by-count":0,"title":["Photochemistry-Based\nDevelopment of Ionizable Lipid\nLibrary for mRNA-Lipid Nanoparticle Delivery In Vivo"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8542-1071","authenticated-orcid":true,"given":"Simin","family":"Chun","sequence":"first","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hyorim","family":"Nam","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Donghyun","family":"Lee","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yeeun","family":"Lee","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheol Hui","family":"Park","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chaehwan","family":"Lim","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Donghyun","family":"Kim","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ji Sun","family":"Park","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kee-Pyo","family":"Kim","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hak Soo","family":"Choi","sequence":"additional","affiliation":[{"name":"ADA Forsyth Institute , , 100 Chestnut St , , ,","place":["Somerville, Massachusetts, United States, 02143"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2193-6583","authenticated-orcid":true,"given":"Heebeom","family":"Koo","sequence":"additional","affiliation":[{"name":"The Catholic University of Korea , , 222 Banpo-Daero , Seocho-Gu, ,","place":["Seoul, Republic of Korea, 06591"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,21]]},"reference":[{"key":"2026100711123304700_cit1","doi-asserted-by":"publisher","first-page":"709","DOI":"10.1038\/s41573-024-00977-6","article-title":"The 60-year evolution of lipid nanoparticles for nucleic\nacid delivery","volume":"23","author":"Cullis","year":"2024","journal-title":"Nat. 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Biotechnol."},{"key":"2026100711123304700_cit43","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-020-16248-y","article-title":"Synergistic\nlipid compositions for\nalbumin receptor mediated delivery of mRNA to the liver","volume":"11","author":"Miao","year":"2020","journal-title":"Nat. Commun."},{"key":"2026100711123304700_cit44","doi-asserted-by":"publisher","first-page":"653","DOI":"10.1038\/nbt.2614","article-title":"Efficiency of siRNA\ndelivery by lipid nanoparticles is limited by\nendocytic recycling","volume":"31","author":"Sahay","year":"2013","journal-title":"Nat. Biotechnol."},{"key":"2026100711123304700_cit45","doi-asserted-by":"publisher","DOI":"10.1186\/s12951-025-03836-7","article-title":"Size control\nof lipid nanoparticles\nvia simulation-based design of microfluidic chip and its effect on\nmRNA delivery in vitro and in vivo","volume":"23","author":"Kim","year":"2025","journal-title":"J. Nanobiotechnol."},{"key":"2026100711123304700_cit46","doi-asserted-by":"publisher","first-page":"44605","DOI":"10.1021\/jacs.5c19387","article-title":"Thioketal-incorporated biodegradable\nlipid nanoparticles deliver mRNA to ductal epithelial cells for improved\npancreatic cancer treatment","volume":"147","author":"Qiu","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026100711123304700_cit47","doi-asserted-by":"publisher","first-page":"872","DOI":"10.1038\/mt.2009.36","article-title":"Development of lipidoid\u2013siRNA\nformulations\nfor systemic delivery to the liver","volume":"17","author":"Akinc","year":"2009","journal-title":"Mol. 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