Making healthy food choices is challenging for many people. Individuals differ greatly in their ability to follow health goals in the face of temptation, but it is unclear what underlies such differences. Using voxel-based morphometry, we investigated in healthy humans (i.e., men and women) the links between structural variation in gray matter volume and individuals' level of success in shifting toward healthier food choices. We combined MRI and choice data into a joint dataset by pooling across three independent studies that used a task prompting participants to explicitly focus on the healthiness of food items before making their food choices. Within this dataset, we found that individual differences in gray matter volume in the ventromedial prefrontal cortex (vmPFC) and dorsolateral prefrontal cortex (dlPFC) predicted regulatory success. We extended and confirmed these initial findings by predicting regulatory success out of sample and across tasks in a second dataset requiring participants to apply a different regulation strategy that entailed distancing from cravings for unhealthy, appetitive foods. Our findings suggest that neuroanatomical markers in the vmPFC and dlPFC generalized to different forms of dietary regulation strategies across participant groups. They provide novel evidence that structural differences in neuroanatomy of two key regions for valuation and its control, the vmPFC and dlPFC, predict an individual's ability to exert control in dietary choices.SIGNIFICANCE STATEMENT Dieting involves regulating food choices to eat healthier foods and fewer unhealthy foods. People differ dramatically in their ability to achieve or maintain this regulation, but it is unclear why. Here, we show that individuals with more gray matter volume in the dorsolateral and ventromedial prefrontal cortex are better at exercising dietary self-control. This relationship was observed across four different studies examining two different forms of dietary self-regulation, suggesting that neuroanatomical differences in the ventromedial prefrontal cortex and dorsolateral prefrontal cortex may represent a general marker for self-control abilities. These results identify candidate neuroanatomical markers for dieting success and failure, and suggest potential targets for therapies aimed at preventing or treating obesity and related eating disorders.