Successful goal pursuit involves repeatedly engaging self-control against temptations or distractions that arise along the way. Laboratory studies have identified the brain systems recruited during isolated instances of self-control, and ecological studies have linked self-control capacity to goal outcomes. However, no study has identified the neural systems of everyday self-control during long-term goal pursuit. The present study integrated neuroimaging and experience-sampling methods to investigate the brain systems of successful self-control among smokers attempting to quit. A sample of 27 cigarette smokers completed a go/no-go task during functional magnetic resonance imaging before they attempted to quit smoking and then reported everyday self-control using experience sampling eight times daily for 3 weeks while they attempted to quit. Increased activation in right inferior frontal gyrus, pre-supplementary motor area, and basal ganglia regions of interest during response inhibition at baseline was associated with an attenuated association between cravings and subsequent smoking. These findings support the ecological validity of neurocognitive tasks as indices of everyday response inhibition.