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Background: Despite the known benefits of physical activity, the prevalence of physical inactivity and sedentary behavior are significant issues in public health. Young adults, such as college students, are a population at risk for decreased physical activity participation due to the newfound responsibility of balancing school, work, and personal responsibilities. Previous findings indicated the lack of motivation was one of the important factors explaining the decreased physical activity participation. The emerging technology of immersive virtual reality combining with exercise provide a fun and motivating means for promoting physical activity and health-related outcomes. The cross-sectional studies have shown the promising influences of immersive virtual reality exercise on health-related outcomes, however, there is no experimental study to further conclude the findings. Therefore, the purpose of this randomized control trial was to examine the effectiveness of a 4-week VR-based exercise intervention on promoting PA and improving physiological and psychological outcomes among college students. Methods: A total of 36 college students were recruited from the University of Minnesota Twin Cities. Participants were randomly assigned to two groups: (1) intervention group – participants were asked to exercise on an immersive virtual reality-based exercise bike for one hour per session, two times per week, for 4 weeks; (2) control group – participants were asked to maintain their usual activities for 4 weeks. Participants’ weight, height, percentage of body fatness, and cardiovascular fitness were assessed by the validated instruments at baseline and 4 weeks. The exercise motivation, mood states, and depressive symptoms were assessed via a battery of surveys at baseline and 4 weeks. Participants’ physical activity levels were assessed via International Physical Activity Questionnaire at baseline and post-intervention follow-up. A two-way repeated measures ANOVA was used to examine the differences between intervention and control group on physiological and psychological outcomes over time. The within-subjects factor was “time” and the between-subjects factor was “group”. Results: The Chi-Square test and the independent t-test indicated that there was no statistically significant difference regarding baseline demographic, physiological, and psychological outcomes between intervention and control group at baseline. Regarding exercise motivation, significant interactions were observed on identified regulation (F(1,34) = 6.55, p = 0.02) and intrinsic regulation (F(1,34) = 11.21, p = 0.02). Regarding mood states, significant interactions were observed on confusion (F(1,34) = 6.72, p = 0.01), fatigue (F(1,34) = 6.46, p = 0.02), tension (F(1,34) = 10.44, p = 0.003), and vigor (F(1,34) = 7.22, p = 0.01). In addition, a significant interaction was observed on the depression symptoms (F(1,34) = 5.53, p = 0.03). Regarding physiological outcomes, significant interactions were observed on percentage of body fatness (F(1,34) = 17.26, p