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Herein, cannabinoid receptor 1 (CB1)\u2010 and reactive oxygen species (ROS)\u2010targeting electrosprayed microspheres (MSs) are fabricated by loading with the CB1 agonist arachidonoyl 2\u2032\u2010chloroethylamide (ACEA) and producing ROS in a photoresponsive manner. The synergistic anti\u2010tumor effects of ACEA and ROS released from the MSs are assessed. ACEA inhibits epidermal growth factor receptor signaling and altered tumor microenvironment (TME) by activating CB1 to induce tumor cell death. The MSs are composed of glycidyl methacrylate\u2010conjugated xanthan gum (XGMA) and Fe<jats:sup>3+<\/jats:sup>, which form dual molecular networks based on a Fe<jats:sup>3+<\/jats:sup>\u2010(COO<jats:sup>\u2212<\/jats:sup>)<jats:sub>3<\/jats:sub> network and a C\u2550C addition reaction network. Interestingly, the Fe<jats:sup>3+<\/jats:sup>\u2010(COO<jats:sup>\u2212<\/jats:sup>)<jats:sub>3<\/jats:sub> network can be disassembled instantly under the conditions of lactate sodium and ultraviolet exposure, and the disassembly is accompanied by massive ROS production, which directly injures tumor cells. Meanwhile, the transition of dual networks to a single network boosts the ACEA release. Together, the activities of the ACEA and MSs promote immunogenic tumor cell death and create a tumor\u2010suppressive TME by increasing M1\u2010like tumor\u2010associated macrophages and CD8<jats:sup>+<\/jats:sup> T cells. In summation, this study demonstrates strong prospects of improving anti\u2010tumor effects of drug delivering platforms through molecular design.<\/jats:p>","DOI":"10.1002\/advs.202308051","type":"journal-article","created":{"date-parts":[[2024,2,13]],"date-time":"2024-02-13T21:19:58Z","timestamp":1707859198000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Molecular Engineering of Electrosprayed Hydrogel Microspheres to Achieve Synergistic Anti\u2010Tumor Chemo\u2010Immunotherapy with ACEA Cargo"],"prefix":"10.1002","volume":"11","author":[{"given":"Youming","family":"Deng","sequence":"first","affiliation":[{"name":"Department of General Surgery Xiangya Hospital International Joint Research Center of Minimally Invasive Endoscopic Technology Equipment and Standards Central South University  Changsha 410008 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