This study examined motivation, positive and negative outcome expectations of quitting, and self-efficacy as predictors of quit attempts and cessation maintenance in a smoking cessation intervention for college students (N = 303). Psychological measures assessed at baseline were used to predict smoking behavior outcomes. Analysis of variance (ANOVA) and logistic regression analysis revealed that motivation and self-efficacy were strong, differential predictors of quit attempts and cessation maintenance, respectively. This study extends the previous findings regarding psychological predictors of quitting processes to college students, and suggests the need for interventions tailored according to phases of quitting processes.