In summary, we found that more dependent smokers experienced greater negative affect and craving at baseline and postquit, regardless of abstinence status. This suggests that those with a predisposition to experience negative affect are prone to greater nicotine dependence, and not that greater nicotine dependence causes greater negative affect and craving during withdrawal. We found no support for the hypothesis that smoking relapse results in greater negative affect and craving than abstinence. Craving was associated with negative affect across measurement modalities. These results highlight the benefits of using multimodal measures to study the impact of nicotine dependence and withdrawal on negative affect and craving.