Smoking tobacco is a major threat to public health, but only a small percentage of smokers succeed in quitting. Given this, extant literature has begun to examine modifiable internal factors, such as impulsivity and self-efficacy, as intervention targets for improving cessation outcomes. The present study examined interrelationships between trait impulsivity, impulsive behavior, and self-efficacy, and the degree to which they predict smoking cessation outcomes in a sample of adult cigarette smokers motivated to quit. Three hypotheses were examined: first, it was expected that behavioral impulsivity would exacerbate the expected negative effects of trait impulsivity on self-efficacy. Second, it was hypothesized that multiple measures of impulsive behavior would exhibit good convergent validity and when combined would serve as a better predictor of cessation outcomes than either measure alone. Finally, it was expected that trait impulsivity’s expected negative effect on smoking cessation would be attenuated by self-efficacy and exacerbated by impulsive behavior.