Nanocatalytic therapy is an emerging technology that utilizes synthesized nanoscale enzyme mimetics for biomedical treatment. However, in the field of neuroscience, achieving neuroprotection while killing tumor cells is a technological challenge. Here, we synthesized a biomimetic and transformed cerium vanadate (CeVO4) nanoenzyme for the treatment of glioblastoma (GBM) and the repair of GBM induced brain injury after ionizing radiation (IR). The system exhibits pH dependence: it exhibits strong superoxide dismutase (SOD) enzyme activity in neutral environments and peroxidase (POD) enzyme activity in acidic environments. In GBM cells, this system functions in lysosomes, leading to cell damage and accumulation of reactive oxygen species (ROS); In neuronal cells, this nanoenzyme can undergo lysosomal escape and aggregate with mitochondrial nanoenzymes, reversing mitochondrial damage caused by IR and restoring the expression level of anti apoptotic BCL-2 protein. Mechanistically, we believe that this distribution difference is related to specific uptake internalization mechanisms and lysosomal repair pathways in neurons, ultimately leading to a dual role of tumor killing and neural repair in vivo models. In summary, this study provides ideas for the repair of brain injury after radiotherapy for glioblastoma.