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Mood and personality-based vulnerabilities have been extensively examined in patients with substance use disorders, but their relevance as models of etiology remains to be fully investigated. The present investigation examined mood and personality-based models of substance use in a nonclinical sample of young adults. Two-hundred and twelve individuals were assessed for personality and clinical characteristics and participated in computerized ambulatory monitoring of mood states and substance use over a 1-week period. Personality factors were strong predictors of substance use frequency over the previous 30 days, as well as of substance use in daily life using ambulatory monitoring. A linear increase was also observed in the intensity of novelty seeking and antisocial personality traits as a function of the social deviance of substances used. However, mood disorder history was related only to the use of illicit drugs other than cannabis, and fluctuations in mood states did not prospectively predict daily use of substances in a manner consistent with self-medication. Moreover, there was little evidence that personality characteristics moderated relations between mood states and substance use in daily life. The relevance of results for mood and personality models of substance use etiology is discussed.