Purpose: Radiation injury is a serious threat to humans that requires prompt and accurate diagnosis and assessment. Currently, there is no effective imaging method to evaluate acute radiation injury in the early stage. We used hybrid multifunctional MRI to evaluate acute radiation-induced brain injury. Materials and methods: Different extents of brain injury were created by exposing SD rats to different radiation doses, namely, 0, 10, 20, 30 and 40 Gy. DCE, IVIM-MRI and MRS were performed on the 5th day after irradiation. Immunohistochemistry, western blotting and electron microscopy were used to determine histopathological changes in neurons and glial cells. Results: The Ktrans, Ve, and iAUC values in DCE and the SO, f and D* values in IVIM showed significant positive correlations with injury grade. In particular, Ktrans, iAUC and SO showed very good correlations with injury grade (r > 0.5, P < 0.05), and the values in the 30 Gy group were significantly higher than those in the other groups (P < 0.05). The NAA/Cr ratio in the 30 Gy group was significantly lower than those in the other groups, whereas the NAA/Cho ratio increased from the 10 Gy to the 20 Gy group and decreased significantly in the 30 Gy group (P < 0.05). VEGF, Caspase-3 and GFAP increased with irradiation dose increasing from 10 Gy to 30 Gy (P < 0.05). ROC analysis demonstrated that multifunctional MRI was more effective for diagnosing the 30 Gy group than it was for the 10 Gy and 20 Gy groups. Conclusion: Hybrid multifunctional MRI can noninvasively evaluate acute radiation -induced brain injury in the early stage, particularly high-dose radiation exposure.