Exercise is consistently related to physical and psychological health benefits in older adults. Bandura’s social-cognitive theory (SCT) is one theoretical perspective on understanding and predicting exercise behavior. Thus, the authors examined whether three SCT variables—self-efficacy, self-regulation, and outcome-expectancy value—predicted older adults’ (N = 98) exercise behavior. Bivariate analyses revealed that regular exercise was associated with being male, White, and married; having higher income, education, and self-efficacy; using self-regulation skills; and having favorable outcome-expectancy values (p < .05). In a simultaneous multivariate model, however, self-regulation (p = .0097) was the only variable independently associated with regular exercise. Thus, exercise interventions targeting older adults should include components aimed at increasing the use of self-regulation strategies.