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Herein, we report a single-component backbone-ionized polymer platform, establishing QSARs for extra-hepatic mRNA expression and providing an ideal model for elucidating the local structural rearrangement mechanisms. By converting the tertiary amines on poly(\u03b2-amino ester) (P\u03b2AE) into quaternary ammonium salts (ionization), we developed ionized P\u03b2AE (iP\u03b2AE) and constructed a platform containing 90 P\u03b2AE variants through tuning the ionization proportion and side-chain chemistry. In vivo screening reveals the QSAR, the differential ionization gradient-induced targeting (DIGIT), which summarizes the side-chain-regulated quantitative relationship between the ionization proportion and the organ-selective expression intensity of mRNA. The rearrangement-mediated affinity control and translation (RE-ACT) mechanism elucidates that side chains act as molecular switches, inducing distinct \u201cElectrostatic Pincer\u201d or \u201cElectrostatic-Hydrogen Tethering\u201d modes, thereby precisely controlling the intracellular release and translation efficiency of mRNA. Furthermore, leveraging the lyophilized formulation of iP\u03b2AE, antigen mRNA (OVA\/MUC1) and p53 mRNA were efficiently delivered to the spleen and lung, respectively. The lifespan of mice was extended by 20 times with vaccine immunotherapy, and chemosensitivity was increased with protein replacement therapy. Collectively, this iP\u03b2AE platform establishes a broadly applicable framework for engineering next-generation mRNA carrier systems.<\/jats:p>","DOI":"10.1021\/jacs.6c11271","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T14:36:39Z","timestamp":1785854199000},"page":"33803-33817","source":"Crossref","is-referenced-by-count":0,"title":["Backbone-Ionized\nPolymers for Quantitatively Guided\nExtra-Hepatic mRNA Expression via Differential Local Structural Rearrangement"],"prefix":"10.1021","volume":"148","author":[{"given":"Yiwan","family":"Geng","sequence":"first","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, PR China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongfang","family":"Zheng","sequence":"additional","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, PR China, 100029"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Yang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, PR China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xianren","family":"Zhang","sequence":"additional","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, PR China, 100029"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenlin","family":"An","sequence":"additional","affiliation":[{"name":"Sinopharm Group , , ,","place":["Beijing, PR China, 101111"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiuheng","family":"Shen","sequence":"additional","affiliation":[{"name":"Sinopharm Group , , ,","place":["Beijing, PR China, 101111"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiyue","family":"Jiao","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, PR China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yusheng","family":"Zhang","sequence":"additional","affiliation":[{"name":"China Academy of Chinese Medical Sciences , , ,","place":["Beijing, PR China, 100700"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6981-7794","authenticated-orcid":true,"given":"Dapeng","family":"Cao","sequence":"additional","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, PR China, 100029"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiguo","family":"Lu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, PR China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4106-0344","authenticated-orcid":true,"given":"Xin","family":"Zhang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, PR China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,3]]},"reference":[{"issue":"11","key":"2026081210090149100_cit1","doi-asserted-by":"publisher","first-page":"1586","DOI":"10.1038\/s41587-022-01491-z","article-title":"Unlocking\nthe Promise of mRNA Therapeutics","volume":"40","author":"Rohner","year":"2022","journal-title":"Nat. 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Cancer Res."},{"issue":"1","key":"2026081210090149100_cit46","doi-asserted-by":"publisher","first-page":"45","DOI":"10.1016\/j.ymthe.2017.10.020","article-title":"Combination Immunotherapy\nof MUC1 mRNA Nano-Vaccine\nand CTLA-4 Blockade Effectively Inhibits Growth of Triple Negative\nBreast Cancer","volume":"26","author":"Liu","year":"2018","journal-title":"Mol. 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