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The release of lipopolysaccharide (LPS) following antibiotic treatment and the resulting proinflammatory cascade necessitate the simultaneous application of effective inflammation management. Herein, a series of selenium\u2010functionalized polypeptides are developed with the reversible redox properties of selenium and positive charge units, having negative antibacterial and anti\u2010inflammatory synchronously. The optimal peptide, PSe\n                    <jats:sub>50<\/jats:sub>\n                    \u2010CF, can effectively kill many Gram\u2010negative bacteria, including\n                    <jats:italic>E. coli<\/jats:italic>\n                    ,\n                    <jats:italic>P. aeruginosa<\/jats:italic>\n                    , and\n                    <jats:italic>A. baumannii<\/jats:italic>\n                    belonging to the ESCAPE family. PSe\n                    <jats:sub>50<\/jats:sub>\n                    \u2010CF disrupts outer membrane integrity and inhibits LPS biosynthesis via dual targeting of LPS and phospholipids and further downregulates critical genes for lipid A biosynthesis and the BamA component of the \u03b2\u2010barrel assembly machinery (BAM complex). Crucially, leveraging selenium's reversible redox and immune regulation properties, PSe\n                    <jats:sub>50<\/jats:sub>\n                    \u2010CF exhibited potent anti\u2010inflammatory effects both in vitro and in vivo by neutralizing LPS and suppressing Toll\u2010like receptor 4 (TLR4) signaling, thereby blocking proinflammatory cytokines. This dual\u2010action mechanism translates to superior therapeutic efficacy in murine models of cecal ligation\/puncture (CLP) sepsis and\n                    <jats:italic>E. coli<\/jats:italic>\n                    \u2010induced peritonitis. Together, these findings position selenium\u2010functionalized polypeptides as a highly promising therapeutic strategy for Gram\u2010negative sepsis therapy and a paradigm for next\u2010generation antimicrobial design.\n                  <\/jats:p>","DOI":"10.1002\/smll.202509805","type":"journal-article","created":{"date-parts":[[2025,11,20]],"date-time":"2025-11-20T14:03:11Z","timestamp":1763647391000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Synergistic Antibacteria and Anti\u2010Inflammation with Reversible Redox Selenium\u2010Functionalized Polypeptides for Efficient Gram\u2010Negative Bacterial Sepsis Treatment"],"prefix":"10.1002","volume":"22","author":[{"given":"Qing","family":"Yu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Polymer Science and Technology Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun 130022 P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziqing","family":"Liang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Polymer Science and Technology Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun 130022 P. R. China"},{"name":"School of Applied Chemistry and Engineering University of Science and Technology of China  Hefei 230026 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia","family":"Hu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Polymer Science and Technology Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun 130022 P. R. China"},{"name":"School of Applied Chemistry and Engineering University of Science and Technology of China  Hefei 230026 P. R. 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