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Delivery of arsenic trioxide (ATO), a clinical anticancer drug, has drawn much attention to improve its pharmacokinetics and bioavailability for efficient cancer therapy.Real-time and in situ monitoring of ATO behaviors in vivo is highly desirable for efficient tumor treatment.Herein,we report an ATO-based multifunctional drug delivery system that efficiently delivers ATO to treat solid tumors and allows real-time monitoring of ATO release by activatable T1 imaging.