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Many clinicians and researchers hypothesize that tobacco use disorders, regardless of the route of administration, are maintained by the ability of nicotine to regulate positive and negative mood states. The present study (N = 137) examined whether certain mood states predicted dependence on either cigarettes or smokeless tobacco and whether specific personality characteristics (e.g., extraversion, neuroticism, and psychoticism) mediated these relationships among young male college students. Results indicated that positive and negative moods predicted cigarette dependence (p values = .01) and that neuroticism partially mediated the relationship between positive affect and cigarette dependence. Exploratory analyses revealed that positive affect also interacted with neuroticism to predict smokeless tobacco dependence (p = .04). Simple effects analyses revealed that this relationship was maintained only among individuals high in neuroticism. Results suggested that dependence on cigarettes and smokeless tobacco among male college students may have different affective correlates and that certain personality characteristics may enhance and explain the effects of mood on tobacco dependence.