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Mitochondria are core regulators of tumor cell homeostasis, and their damage has become an arresting therapeutic modality against cancer. Despite the development of many mitochondrial‐targeted pharmaceutical agents, the exploration of more powerful and multifunctional medications is still underway. Herein, oxygen vacancy‐rich BiO2‐x wrapped with CaCO3 (named BiO2‐x@CaCO3/PEG, BCP) is developed for...