Objectives: To assess the effects of a 12-week pedometer-based intervention on the physical activity behavior, health-related quality of life (HRQOL), and psychological well-being of first-year university students. Participants: First-year university students (N = 184) were recruited during September 2012 and randomly assigned to an intervention or a control group. Methods: Intervention participants were provided with a pedometer, monthly tracking logs, and follow-up e-mails. Control participants received no intervention. Physical activity, HRQOL, and psychological well-being were measured at baseline and post intervention. Data were analyzed using multivariate/univariate analysis of variance (MANOVA/ANOVA). Results: All participants experienced an increase in mild physical activity (p < 0.01) from baseline to follow-up. The intervention failed to produce significant differences between groups for physical activity (p = 0.28), HRQOL (p = 0.80), or psychological well-being (p = 0.72). Psychological well-being (p < 0.001), vigorous physical activity (p = 0.04), and mental health status (p < 0.001) decreased across the duration of the study. Conclusions: More intensive interventions may be required to elicit physical activity behavior change.