Although many smokers try to quit, relatively few are successful in their attempts. Here we investigated whether the ability to quit smoking is related to behavioral and neural measures of cognitive control. A functional magnetic resonance imaging study with a counting Stroop task was used to measure cognitive control in ex-smokers (. N=10) who had successfully quit smoking and smokers (. N=10) who continuously failed to quit smoking. Behavioral results showed a significant Stroop effect in ex-smokers and smokers. Ex-smokers exhibited less Stroop interference, indicating superior cognitive control compared with smokers. Furthermore, when incongruent trials were contrasted with congruent trials, ex-smokers showed stronger BOLD activity than smokers in the right superior frontal gyrus and anterior cingulate cortex. Although the present study does not permit us to draw strong conclusions regarding causality, the results suggest that successful smoking cessation may be mediated by superior cognitive control.