This exploratory experiment tested the effect of two Virtual Reality (VR) relaxation interventions on measures of physiological arousal and affect, compared to a control. Forty-nine participants were randomly assigned to one of three conditions, all using the Oculus Rift. Participants wore a heart rate (HR) monitor and completed pre- and post-test surveys, including the Positive and Negative Affect Schedule (PANAS), Likert-type, and open feedback questions. Mixed repeated measures ANOVAs revealed significant reductions in HR and affect over time across all conditions, with a significant interaction identified for the breathing condition’s effect on negative affect. Participants were able to identify feeling relaxation, as well as influencing factors. Further, the majority expected, and supported, the introduction of VR interventions in their workplace and/or college, with privacy being a common concern. These results demonstrate the potential of VR augmented relaxation interventions with recommendations for further study provided.