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Failure of antibiotics in resistant infections leads to more effective alternative therapies, like spatiotemporally controllable piezodynamic therapy (PZDT) with deep penetration. Currently, PZDT demands further investigation for improved treatment outcomes and the corresponding therapeutic mechanisms. Herein, a nanocomposite cloaked is reported with a biomimetic coating of TLR\u2010upregulated macrophage membrane for targeted PZDT against MRSA\u2010induced skin wound infection and osteomyelitis, representing surficial and deep infection models, respectively. To boost the therapeutic efficacy, crystal defect engineering is applied by impregnating Fe\n                    <jats:sup>2+<\/jats:sup>\n                    into bismuth oxy\u2010iodide nanosheets to increase the crystal defects. This results in a significantly higher piezoelectric coefficient than in previous reports, contributing to an amplified reactive oxygen species generation for bacterial killing. More importantly, the notable piezoelectric effect not only re\u2010programs the macrophages into an\u00a0anti\u2010inflammatory M2 phenotype for accelerating bacterial wound healing but also stimulates the opening of the piezo\u2010stimulated Ca\n                    <jats:sup>2+<\/jats:sup>\n                    channels and boosts the differentiation of mesenchymal stem cells into osteoblasts for expediting bone tissue repair in osteomyelitis model. Moreover, the Fe\u2010doping supplements T2\u2010magnetic resonance imaging for real\u2010time visualization of nanocomposite distribution. This theranostic system opens a new avenue for future treatment of drug\u2010resistant bacteria\u2010caused diseases.\n                  <\/jats:p>","DOI":"10.1002\/smll.202411906","type":"journal-article","created":{"date-parts":[[2025,1,30]],"date-time":"2025-01-30T01:35:42Z","timestamp":1738200942000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":39,"title":["Defect\u2010Engineered Biomimetic Piezoelectric Nanocomposites With Enhanced ROS Production, Macrophage Re\u2010polarization, and Ca\n                    <sup>2+<\/sup>\n                    Channel Activation for Therapy of MRSA\u2010Infected Wounds and Osteomyelitis"],"prefix":"10.1002","volume":"21","author":[{"given":"Shubham","family":"Roy","sequence":"first","affiliation":[{"name":"School of Science Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application Harbin Institute of Technology  Shenzhen 518055 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