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Despite the development of many mitochondrial\u2010targeted pharmaceutical agents, the exploration of more powerful and multifunctional medications is still underway. Herein, oxygen vacancy\u2010rich BiO<jats:sub>2\u2010x<\/jats:sub> wrapped with CaCO<jats:sub>3<\/jats:sub> (named BiO<jats:sub>2\u2010x<\/jats:sub>@CaCO<jats:sub>3<\/jats:sub>\/PEG, BCP) is developed for full\u2010fledged attack on mitochondrial function. After endocytosis of BCP by tumor cells, the CaCO<jats:sub>3<\/jats:sub> shell can be decomposed in the acidic lysosomal compartment, leading to immediate Ca<jats:sup>2+<\/jats:sup> release and CO<jats:sub>2<\/jats:sub> production in the cytoplasm. Near\u2010infrared irradiation enhances the adsorption of CO<jats:sub>2<\/jats:sub> onto BiO<jats:sub>2\u2010x<\/jats:sub> defects, which enables highly efficient photocatalysis of CO<jats:sub>2<\/jats:sub>\u2010to\u2010CO. Meanwhile, such BiO<jats:sub>2\u2010x<\/jats:sub> nanosheets possess catalase\u2010, peroxidase\u2010 and oxidase\u2010like catalytic activities under acidic pH conditions, allowing hypoxia relief and the accumulation of diverse reactive oxygen species (ROS) in the tumor microenvironment. Ca<jats:sup>2+<\/jats:sup> overload\u2010induced ion dyshomeostasis, CO\u2010mediated respiratory chain poisoning, ROS\u2010triggered oxidative stress aggravation, and cytosolic hyperoxia can cause severe mitochondrial disorders, which further lead to type I cell death in carcinoma. Not only does BCP cause irreversible apoptosis, but immunogenic cell death is simultaneously triggered to activate antitumor immunity for metastasis inhibition. Collectively, this platform promises high benefits in malignant tumor therapy and may expand the medical applications of bismuth\u2010based nanoagents.<\/jats:p>","DOI":"10.1002\/smll.202307404","type":"journal-article","created":{"date-parts":[[2023,12,6]],"date-time":"2023-12-06T19:26:24Z","timestamp":1701890784000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Vacancy\u2010Rich Bismuth\u2010Based Nanosheets for Mitochondrial Destruction via CO Poisoning, Ca<sup>2+<\/sup> Dyshomeostasis, and Oxidative Damage"],"prefix":"10.1002","volume":"20","author":[{"given":"Yinmin","family":"Zhao","sequence":"first","affiliation":[{"name":"School of Materials and Energy Southwest University  Chongqing 400715 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoqin","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Materials and Energy Southwest University  Chongqing 400715 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