Many studies have linked activity in a frontostriatal network with the capacity to suppress inappropriate thoughts and actions, but relatively few have examined the role of connectivity between these structures. Here, we use diffusion tensor imaging to assess frontostriatal connectivity in 21 subjects (ages 7-31 years). Fifteen subjects were tested on a go/no-go task, where they responded with a button press to a visual stimulus and inhibited a response to a second infrequent stimulus. An automated fiber tracking algorithm was used to delineate white matter fibers adjacent to ventral prefrontal cortex and the striatum, and the corticospinal tract, which was not expected to contribute to control per se. Diffusion in frontostriatal and corticospinal tracts became more restricted with age. This shift was paralleled by an increase in efficiency of task performance. Frontostriatal radial diffusivities predicted faster reaction times, independent of age and accuracy, and this correlation grew stronger for trials expected to require greater control. This was not observed in the corticospinal tract. On trials matched for speed of task performance, adults were significantly more accurate, and accuracies were correlated with frontostriatal, but not corticospinal, diffusivities. These findings suggest that frontostriatal connectivity may contribute to developmental and individual differences in the efficient recruitment of cognitive control.