The present study used brain imaging to determine the neural basis of individual differences in multitasking, the ability to successfully perform at least two attention-demanding tasks at once. Multitasking is mentally taxing and, therefore, should recruit the prefrontal cortex to maintain task goals when coordinating attentional control and managing the cognitive load. To investigate this possibility, we used functional neuroimaging to assess neural activity in both extraordinary multitaskers (Supertaskers) and control subjects who were matched on working memory capacity. Participants performed a challenging dual N-back task in which auditory and visual stimuli were presented simultaneously, requiring independent and continuous maintenance, updating, and verification of the contents of verbal and spatial working memory. With the task requirements and considerable cognitive load that accompanied increasing N-back, relative to the controls, the multitasking of Supertaskers was characterized by more efficient recruitment of anterior cingulate and posterior frontopolar prefrontal cortices. Results are interpreted using neuropsychological and evolutionary perspectives on individual differences in multitasking ability and the neural correlates of attentional control.