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A smart self‐assembled US/GSH dual‐responsive nanovesicle was synthesized by self‐assembly of Janus Au‐MnO NP. It could be consecutively disassembled into the small Janus Au‐MnO NPs and smaller Au NPs and Mn2+ for dual MRI/PAI‐guided synergistic sono‐chemodynamic therapy. Abstract. Sonodynamic therapy (SDT) has the advantages of high penetration, non‐invasiveness, and controllability, and it is suitable for deep‐seated tumors. However, there is still a lack of effective sonosensitizers with high sensitivity, safety, and penetration. Now, ultrasound (US) and glutathione (GSH) dual responsive vesicles of Janus Au‐MnO nanoparticles (JNPs) were coated with PEG and a ROS‐sensitive polymer. Upon US irradiation, the vesicles were disassembled into

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