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The level of tumor killing by bismuth nanoparticles (BiNPs) as radiosensitizers depends strongly on the powerful particle−matter interaction. However, this same radiation leads to the structural damage in BiNPs, consequently weakening their specific physicochemical properties for radiosensitization. Herein, we studied the radiation-induced corrosion behavior of BiNPs and demonstrated that these damages were manifested by the change in their morphology and crystal structure as well as self-oxidation at their surface. Furthermore, artificial heterostructures were created with graphene nanosheets to greatly suppress the radiation-induced corrosion in BiNPs and enhance their radiocatalytic activity for radiotherapy enhancement. Such a nanocomposite allows the accumulation of overexpressed glutathione, a natural hole scavenger, at the reaction interfaces. This enables the rapid removal of radiogenerated holes from the surface of BiNPs and minimizes the self-radiooxidation, therefore resulting in an efficient suppression of radiation corrosion and a decrease of the depletion of reactive oxygen species (ROS). Meanwhile, the radioexcited conduction band electrons react with the high-level H 2 O 2 within cancer cells to yield more ROS, and the secondary electrons are trapped by H 2 O molecules to produce hydrated electrons capable of reducing a highly oxidized species such as cytochrome c. These radiochemical reactions together with hyperthermia can regulate the tumor microenvironment and accelerate the onset of cellular redox disequilibrium, mitochondrial dysfunction, and DNA damage, finally triggering tumor apoptosis and death. The current work will shed light on radiosensitizers with an enhanced corrosion resistance for controllable and synergistic radio-phototherapeutics.