Functional neuroimaging studies have identified brain regions associated with human taste perception, but only a few have investigated the associations with brain structure. Here, in this exploratory study, we examined the association between the volumes of 82 regions of interest (ROI) and the perceived intensities of sweet (a weighted mean rating of glucose, fructose, aspartame, neohesperidin dihydrochalcone) and bitter (propylthiouracil, quinine, caffeine) substances in a large Australian healthy cohort from the Queensland Twin IMaging (QTIM, n = 559) study and the perceived intensity of quinine in a large U.S. healthy cohort from the Human Connectome Project (HCP, n = 1101). In QTIM, the volumes of 3 cortical (right cuneus gyrus, left transverse temporal gyrus, right inferior temporal gyrus) and one subcortical structure (both left and right caudate) were associated with more than one taste stimulus (P < 0.05) and tended to be associated with both sweet and bitter tastes in the same direction, suggesting these ROIs were more broadly tuned for taste sensation. A further 11 ROIs were associated with a specific taste (sweetness: 4; propylthiouracil: 3; caffeine: 2; quinine: 2). In HCP, volumes of 5 ROIs were associated with quinine bitterness. The quinine-left entorhinal cortex association was found in both QTIM (r = -0.12, P = 3.7 × 10−3) and HCP (r = -0.06, P = 2.0 × 10−2). This study provides the first evidence that, even in healthy people, variation in brain structure is associated with taste intensity ratings, and provides new insights into the brain gustatory circuit.