Attentional deployment is an emotion regulation strategy that involves shifting attentional focus towards or away from particular aspects of emotional stimuli. Previous studies have highlighted the prevalence of attentional deployment and demonstrated that it can have a significant impact on brain activity and behavior. However, little is known about the neural correlates of this strategy. The goal of the present studies was to examine the effect of attentional deployment on neural activity by directing attention to more or less arousing portions of unpleasant images. In Studies 1 and 2, participants passively viewed counterbalanced blocks of unpleasant images without a focus, unpleasant images with an arousing focus, unpleasant images with a non-arousing focus, neutral images without a focus, and neutral images with a non-arousing focus for 4000ms each. In Study 2, eye-tracking data was collected on all participants during image acquisition. In both studies, affect ratings following each block indicated that participants felt significantly less negative affect after viewing unpleasant images with a non-arousing focus compared to unpleasant images with an arousing focus. In both studies, the unpleasant non-arousing focus condition compared to the unpleasant arousing focus condition was associated with increased activity in frontal and parietal regions implicated in inhibitory control and visual attention. In Study 2, the unpleasant non-arousing focus condition compared to the unpleasant arousing focus condition was associated with reduced activity in the amygdala and visual cortex. Collectively these data suggest that attending to a non-arousing portion of an unpleasant image successfully reduces subjective negative affect and recruits fronto-parietal networks implicated in inhibitory control. Moreover, when ensuring task compliance by monitoring eye movements, attentional deployment modulates amygdala activity.