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Achieving much higher selectivity of AMPs towards bacteria and normal cells has always been a continuous goal to be pursued. Herein, a series of sulfonium\u2010based polypeptides with different degrees of branching and polymerization were synthesized by mimicking the structure of vitamin U. The polypeptide, G\n                    <jats:sub>2<\/jats:sub>\n                    \u2010PM\u20101\n                    <jats:sup>H+<\/jats:sup>\n                    , shows both potent antibacterial activity and the highest selectivity index of 16000 among the reported AMPs or peptoids (e.g., the known index of 9600 for recorded peptoid in\n                    <jats:italic>\u201cAngew. Chem. Int. Ed<\/jats:italic>\n                    ., 2020, 59, 6412.\u201d), which can be attributed to the high positive charge density of sulfonium and the regulation of hydrophobic chains in the structure. The antibacterial mechanisms of G\n                    <jats:sub>2<\/jats:sub>\n                    \u2010PM\u20101\n                    <jats:sup>H+<\/jats:sup>\n                    are primarily ascribed to the interaction with the membrane, production of reactive oxygen species (ROS), and disfunction of ribosomes. Meanwhile, altering the degree of alkylation leads to selective antibacteria against either gram\u2010positive or gram\u2010negative bacteria in a mixed\u2010bacteria model. Additionally, both in vitro and in vivo experiments demonstrated that G\n                    <jats:sub>2<\/jats:sub>\n                    \u2010PM\u20101\n                    <jats:sup>H+<\/jats:sup>\n                    exhibited superior efficacy against methicillin\u2010resistant\n                    <jats:italic>Staphylococcus aureus<\/jats:italic>\n                    (MRSA) compared to vancomycin. Together, these results show that G\n                    <jats:sub>2<\/jats:sub>\n                    \u2010PM\u20101\n                    <jats:sup>H+<\/jats:sup>\n                    possesses high biocompatibility and is a potential pharmaceutical candidate in combating bacteria significantly threatening human health.\n                  <\/jats:p>","DOI":"10.1002\/anie.202318011","type":"journal-article","created":{"date-parts":[[2023,12,22]],"date-time":"2023-12-22T08:50:31Z","timestamp":1703235031000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":41,"title":["Structural Element of Vitamin U\u2010Mimicking Antibacterial Polypeptide with Ultrahigh Selectivity for Effectively Treating MRSA Infections"],"prefix":"10.1002","volume":"63","author":[{"given":"Zhenyan","family":"Zhang","sequence":"first","affiliation":[{"name":"School of Applied Chemistry and Engineering University of Science and Technology of China  Hefei 230026 P. 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