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However, its practical application is still suffering from the decreased function and inadequate infiltration of NK cells in the immunosuppressive microenvironment of solid tumors. Herein, we construct light\u2010responsive porphyrin Fe array\u2010armed NK cells (denoted as NK@p\u2010Fe) for cell behavior modulation via bioorthogonal catalysis. By installing cholesterol\u2010modified porphyrin Fe molecules on the NK cell surface, a catalytic array with light\u2010harvesting capabilities is formed. This functionality transforms NK cells into cellular factories capable of catalyzing the production of active agents in a light\u2010controlled manner. NK@p\u2010Fe can generate the active antineoplastic drug doxorubicin through bioorthogonal reactions to enhance the cytotoxic function of NK cells. Beyond drug synthesis, NK@p\u2010Fe can also bioorthogonally catalyze the production of the FDA\u2010approved immune agonist imiquimod (IMQ). The activated immune agonist plays a dual role, inducing dendritic cell maturation for NK cell activation and reshaping the tumor immunosuppressive microenvironment for NK cell infiltration. This work represents a paradigm for the modulation of adoptive cell behaviors to boost cancer immunotherapy by bioorthogonal catalysis.<\/jats:p>","DOI":"10.1002\/anie.202411905","type":"journal-article","created":{"date-parts":[[2024,8,8]],"date-time":"2024-08-08T01:59:55Z","timestamp":1723082395000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Light\u2010Controlled Bioorthogonal Chemistry Altered Natural Killer Cell Activity for Boosted Adoptive Immunotherapy"],"prefix":"10.1002","volume":"63","author":[{"given":"Zhengwei","family":"Liu","sequence":"first","affiliation":[{"name":"Laboratory of Chemical Biology and State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun, Jilin 130022 China"},{"name":"University of Science and Technology of China  Hefei, Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenting","family":"Zhang","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology and State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun, Jilin 130022 China"},{"name":"University of Science and Technology of China  Hefei, Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huisi","family":"Zhao","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology and State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun, Jilin 130022 China"},{"name":"University of Science and Technology of China  Hefei, Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengyu","family":"Sun","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology and State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun, Jilin 130022 China"},{"name":"University of Science and Technology of China  Hefei, Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuanqi","family":"Zhao","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology and State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun, Jilin 130022 China"},{"name":"University of Science and Technology of China  Hefei, Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinsong","family":"Ren","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology and State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun, Jilin 130022 China"},{"name":"University of Science and Technology of China  Hefei, Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2868-3205","authenticated-orcid":false,"given":"Xiaogang","family":"Qu","sequence":"additional","affiliation":[{"name":"Laboratory of Chemical Biology and State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry Chinese Academy of Sciences  Changchun, Jilin 130022 China"},{"name":"University of Science and Technology of China  Hefei, Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,10,14]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaa4967"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/nrc2355"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41568-022-00491-0"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/ni.3518"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202202603"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202002145"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41577-018-0061-z"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.3c02049"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202002780"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1182\/blood.2020007748"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.3390\/cancers15010117"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1126\/scisignal.aai9062"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.1911678117"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00484"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.trechm.2021.11.008"},{"key":"e_1_2_7_16_1","author":"Liu Z.","year":"2023","journal-title":"Angew. 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