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In this study, we introduce a new strategy using protein\u2010integrated hydrogen\u2010bonded organic frameworks (HOFs) to enable synergistic bioorthogonal chemical catalysis and enzymatic catalysis within mitochondria. Utilizing catalytically active tris(4,4\u2032\u2010dicarboxylicacid\u20102,2\u2032\u2010bipyridyl) ruthenium(II) to self\u2010assemble with [1,1\u2032\u2010biphenyl]\u20104,4\u2032\u2010biscarboximidamide, we synthesized nanoscale <jats:bold>RuB\u2010HOFs<\/jats:bold> that exhibit high photocatalytic reduction activity. Notably, <jats:bold>RuB\u2010HOFs<\/jats:bold> efficiently enter cells and preferentially localize to mitochondria, where they facilitate bioorthogonal photoreduction reactions. Moreover, we show that <jats:bold>RuB\u2010HOFs<\/jats:bold> encapsulating catalase can produce hydrogen sulfide (H<jats:sub>2<\/jats:sub>S) in mitochondria through photocatalytic reduction of pro\u2010H<jats:sub>2<\/jats:sub>S and degrade hydrogen peroxide through enzymatic catalysis simultaneously, offering a significant neuroprotective effect against oxidative stress. Our findings not only introduce a versatile chemical toolset for mitochondria\u2010targeted bioorthogonal catalysis for prodrug activation but also pave the way for potential therapeutic applications in treating diseases related to cellular oxidative stress.<\/jats:p>","DOI":"10.1002\/anie.202312784","type":"journal-article","created":{"date-parts":[[2023,10,11]],"date-time":"2023-10-11T07:28:23Z","timestamp":1697009303000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":41,"title":["Neuroprotective Bioorthogonal Catalysis in Mitochondria Using Protein\u2010Integrated Hydrogen\u2010Bonded Organic Frameworks"],"prefix":"10.1002","volume":"62","author":[{"given":"Jiakang","family":"Tang","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Analytical Chemistry for Living Biosystems Institute of Chemistry Chinese Academy of Sciences  100190 Beijing China"},{"name":"University of Chinese Academy of Sciences  100049 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ji","family":"Liu","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Analytical Chemistry for Living Biosystems Institute of Chemistry Chinese Academy of Sciences  100190 Beijing China"},{"name":"University of Chinese Academy of Sciences  100049 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qizhen","family":"Zheng","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Analytical Chemistry for Living Biosystems Institute of Chemistry Chinese Academy of Sciences  100190 Beijing China"},{"name":"University of Chinese Academy of Sciences  100049 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Yao","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Analytical Chemistry for Living Biosystems Institute of Chemistry Chinese Academy of Sciences  100190 Beijing China"},{"name":"University of Chinese Academy of Sciences  100049 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2783-9426","authenticated-orcid":false,"given":"Ming","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Analytical Chemistry for Living Biosystems Institute of Chemistry Chinese Academy of Sciences  100190 Beijing China"},{"name":"University of Chinese Academy of Sciences  100049 Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,10,23]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature12985"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201915826"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.addr.2020.09.010"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apsb.2022.03.001"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.bioadv.2022.212876"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c00188"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201911508"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c12330"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202004379"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202009888"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202008624"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-26655-4"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201901699"},{"key":"e_1_2_7_14_1","first-page":"1","volume":"50","author":"Kang Y. 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