Creative persons play an important role in technical innovation and social progress. There is little research on the neural correlates with researchers with high academic achievement. We used a combined structural (regional gray matter volume, rGMV) and functional (resting-state functional connectivity analysis, rsFC) approach to examine the neural substrates of high academic achievement professors (HAP; compared to low academic achievement professors, LAP). Results showed that HAP had greater rGMV in the left inferior frontal gyrus (mainly in the posterior orbital frontal gyrus, OFG) and supplementary motor cortex (SMA), which might be associated with effective behavioral and cognitive planning and execution; smaller rGMV in the right medial prefrontal gyrus (mPFC) and right inferior parietal lobule (IPL), which might be related to increased novelty seeking and hypothetical thinking. Functional connectivity analysis revealed interactions between some specific brain regions in HAP when the left OFG, the left SMA, and the left postcentral gyrus (PCG) were used as seed regions, which indicated that the interactions between these brain regions might be critically involved in professors' intellectual and creative abilities. Interestingly, the strength rsFC between the left PCG and the right lentiform nucleus was negatively correlated with composite achievement index (smaller number indicates higher academic achievement), which might help to facilitate action planning and execution.