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Here, this work develops a strategy using novel trimethylamine N\u2010oxide (TMAO)\u2010derived zwitterionic hydrogel to promote diabetic wound healing, and explore the multi\u2010cellular ecosystem around zwitterionic hydrogel, mapping out an overview of different cells in the zwitterionic microenvironment by single\u2010cell RNA sequencing. The diverse cellular heterogeneity is revealed, highlighting the critical role of macrophage and neutrophils in managing diabetic wound healing. It is found that polyzwitterionic hydrogel can upregulate <jats:italic>Ccl3+<\/jats:italic> macrophages and downregulate <jats:italic>S100a9+<\/jats:italic> neutrophils and facilitate their interactions compared with polyanionic and polycationic hydrogels, validating the underlying effect of zwitterionic microenvironment on the activation of adaptive immune system. Moreover, zwitterionic hydrogel inhibits the formation of neutrophil extracellular traps (NETs) and promotes angiogenesis, thus improving diabetic wound healing. These findings expand the horizons of the sophisticated orchestration of immune systems in zwitterion\u2010directed diabetic wound repair and uncover new strategies of novel immunoregulatory biomaterials.<\/jats:p>","DOI":"10.1002\/adma.202402738","type":"journal-article","created":{"date-parts":[[2024,6,17]],"date-time":"2024-06-17T20:09:01Z","timestamp":1718654941000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":42,"title":["Tracing Immunological Interaction in Trimethylamine N\u2010Oxide Hydrogel\u2010Derived Zwitterionic Microenvironment During Promoted Diabetic Wound Regeneration"],"prefix":"10.1002","volume":"36","author":[{"given":"Zheng","family":"Li","sequence":"first","affiliation":[{"name":"Department of Prosthodontics Peking University School and Hospital of Stomatology  Beijing 100081 China"},{"name":"National Center for Stomatology &amp; National Clinical Research Center for Oral Diseases &amp; National Engineering Research Center of Oral Biomaterials and Digital Medical Devices &amp; Beijing Key Laboratory of Digital Stomatology &amp; NHC Key Laboratory of Digital Stomatology  22 Zhongguancun South Avenue, Haidian District Beijing 100081 P. 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