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However, compared to ionizable lipids, sterols remain a relatively underexplored design axis. This study discusses the engineering of a library of nine bile acid\u2010derived sterols with different hydroxylation patterns and alkyl tail lengths, and systematically maps how sterol structure governs formulation\u2010level properties and organ\u2010level expression profiles. After integrating physicochemical characterization with all\u2010atom molecular dynamics (MD) simulations, the experimentally observed formulation behaviors correlate with MD\u2010derived membrane structural descriptors. These descriptors provide a quantitative evaluation framework for prioritizing sterol chemotypes based on their predicted encapsulation performance and membrane organization, supporting the notion that sterol\u2010dependent membrane organization provides a structural basis for formulation properties, including mRNA encapsulation. Moreover, substituting cholesterol with bile acid\u2010derived sterols consistently attenuated hepatic expression and shifted organ\u2010level expression toward spleen\u2010dominant profiles, which is central to immune priming and adaptive immune activation. Among bile acid\u2010derived sterols, CA\u201020 LNPs functionally enhance antigen\u2010specific humoral immunity and elicit antigen\u2010specific cellular immune responses, including improved memory\u2010associated immune features, while maintaining an acute safety profile. Collectively, these results establish sterol engineering as a powerful design strategy for modulating LNP formulation properties, in vivo fate, and immunological function.<\/jats:p>","DOI":"10.1002\/advs.76671","type":"journal-article","created":{"date-parts":[[2026,7,21]],"date-time":"2026-07-21T12:15:16Z","timestamp":1784636116000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Molecular Dynamics\u2010Guided Sterol Engineering of mRNA\u2010Lipid Nanoparticles Reprograms Biodistribution and Enhances Spleen\u2010Selective Immunity"],"prefix":"10.1002","volume":"13","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-0999-8906","authenticated-orcid":false,"given":"Sanghyuk","family":"Jeon","sequence":"first","affiliation":[{"name":"Department of Medical and Biological Sciences The Catholic University of Korea  Bucheon Republic of Korea"},{"name":"BK Four Department of Biotechnology The Catholic University of Korea  Bucheon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9037-5361","authenticated-orcid":false,"given":"Seo\u2010Hyeon","family":"Bae","sequence":"additional","affiliation":[{"name":"Department of Medical and Biological Sciences The Catholic University of Korea  Bucheon Republic of Korea"},{"name":"BK Four Department of Biotechnology The Catholic University of Korea  Bucheon Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8935-7852","authenticated-orcid":false,"given":"Jungyong","family":"Ji","sequence":"additional","affiliation":[{"name":"MolCube Inc.  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