There is a long-standing interest in exploring the factors related to student achievement. As a newly explored personality trait, grit is defined as a person's tendency to pursue long-term goals with continual perseverance and passion, and grit plays a critical role in student achievement. Increasing evidence has shown that growth mindset, the belief that one's basic abilities are malleable and can be developed through effort, is a potential factor for cultivating grit. However, less is known about the association between grit and the brain and the role of growth mindset in this association. Here, we utilized voxel-based morphometry to examine the neuroanatomical correlates of grit in 231 healthy adolescent students by performing structural magnetic resonance imaging. The whole-brain regression analyses revealed that the regional gray matter volume (rGMV) in the left dorsolateral prefrontal cortex (DLPFC) negatively predicted grit. In contrast, the rGMV in the right putamen positively predicted grit. Furthermore, mediating analyses suggested that growth mindset served as a mediator in the association between left DLPFC volume and grit. Our results persisted even after controlling for the influences of self-control and delayed gratification. Overall, our study presents novel evidence for the neuroanatomical basis of grit and highlights that growth mindset might play an essential role in cultivating a student's grit level.