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Herein, polyprodrug antimicrobials are proposed to mimic antimicrobial peptides appended with a concurrent drug release property, exhibiting broad\u2010spectrum antibacterial activity and especially high potency to inhibit methicillin\u2010resistant <jats:italic>Staphylococcus aureus<\/jats:italic> (MRSA) without inducing resistance. Two series of polyprodrug antimicrobials are fabricated by facile polymerization of triclosan prodrug monomer (TMA) and subsequent quaternization of hydrophilic poly(<jats:italic>N<\/jats:italic>,<jats:italic>N<\/jats:italic>\u2010dimethylaminoethyl methacrylate) (PDMAEMA), affording PDMAEMA\u2010<jats:italic>b<\/jats:italic>\u2010PTMA and PQDMA\u2010<jats:italic>b<\/jats:italic>\u2010PTMA, respectively. Optimized samples with proper hydrophobic ratio are screened out, which exhibit remarkable bacterial inhibition and low hemolysis toward red blood cells. Furthermore, synergistic antibacterial mechanisms contribute to the bacteria killing, including serious membrane damage, increased out\u2010diffusion of cytosolic milieu across the membrane, and intracellular reductive milieu\u2010mediated triclosan release. No detectable resistance is observed for polyprodrug antimicrobials against MRSA, which is demonstrated to be better than commercial triclosan and vancomycin against in vivo MRSA\u2010infected burn models and a promising approach to the hurdle of antibiotic resistance in biomedicine.<\/jats:p>","DOI":"10.1002\/smll.201802008","type":"journal-article","created":{"date-parts":[[2018,8,17]],"date-time":"2018-08-17T20:24:14Z","timestamp":1534537454000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":67,"title":["Polyprodrug Antimicrobials: Remarkable Membrane Damage and Concurrent Drug Release to Combat Antibiotic Resistance of Methicillin\u2010Resistant <i>Staphylococcus aureus<\/i>"],"prefix":"10.1002","volume":"14","author":[{"given":"Bing","family":"Cao","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Laser Life Science and Institute of Laser Life Science South China Normal University  Guangzhou 510631 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