Background: Previous studies have identified brain areas related to cognitive abilities and personality, respectively. In this exploratory study, we extend the application of modern neuroimaging techniques to another area of individual differences, vocational interests, and relate the results to an earlier study of cognitive abilities salient for vocations. Findings. First, we examined the psychometric relationships between vocational interests and abilities in a large sample. The primary relationships between those domains were between Investigative (scientific) interests and general intelligence and between Realistic (blue-collar) interests and spatial ability. Then, using MRI and voxel-based morphometry, we investigated the relationships between regional gray matter volume and vocational interests. Specific clusters of gray matter were found to be correlated with Investigative and Realistic interests. Overlap analyses indicated some common brain areas between the correlates of Investigative interests and general intelligence and between the correlates of Realistic interests and spatial ability. Conclusions: Two of six vocational-interest scales show substantial relationships with regional gray matter volume. The overlap between the brain correlates of these scales and cognitive-ability factors suggest there are relationships between individual differences in brain structure and vocations.