This study investigated the neural basis of social adjustment using multimodal brain imaging and social-adjustment measurements to analyze functional and structural brain features during social adjustment in college students. The results showed that, regarding brain function, some dimensions of social adjustment were associated with the insula, and some regions of the frontal and occipital lobes. Self-adjustment and satisfaction required activation of the middle frontal gyrus, while career adjustment and academic adjustment required inhibition of the inferior frontal gyrus and lingual gyrus, respectively. Decreased metabolic activity of the lingual gyrus was beneficial for obtaining satisfaction. Regarding brain structure, the total score and some dimensions of social adaptation were associated with the gray matter of portions of the temporal and parietal lobes. The superior temporal gyrus was associated with the total social adjustment and satisfaction score, the middle temporal gyrus with campus-life adjustment and satisfaction, and the post central gyrus and the inferior parietal lobule with emotional adjustment. The changes in the gray matter volume of these brain regions to a certain extent reflected socially adaptive behaviors. The results suggest that social adaptability is associated with various brain regions dispersed among both hemispheres of the brain, and requires synergistic inter-actions between multiple brain regions and both brain hemispheres.