For many smokers, the motivational state of craving is a central feature of their dependence on nicotine, and is often at odds with a general desire to quit. How this desire to quit may influence the craving for a cigarette, however, is unclear. In the current study, we manipulated the level of craving in 24 regular smokers, and recorded EEG measures of brain activity during a rare target detection task utilizing addiction-unrelated stimuli. In response to the non-targets, we observed that smokers wanting to quit showed an enhanced late frontal activation when they were craving vs. not craving, whereas smokers not wanting to quit showed the opposite pattern of activity. A dissociation was also present in the target-related P300 response as a function of craving and desire to quit, with smokers who did not want to quit processing targets differentially between the states of craving and non-craving. The data suggest that distinct top-down control mechanisms during craving may be implemented by people who wish to quit smoking, as compared to those who do not wish to quit. This pattern of findings establishes this ERP activity as a potential biomarker that may help to differentiate people who want to quit their addiction from those who wish to continue to use their substance of choice.