It is understood that in order for athletes to perform to their potential consistently they must learn to optimally self-regulate their psychological and physiological states. Yet, the process by which this is accomplished is not well understood. The purpose of this doctoral dissertation was to explore the concept of self-regulation in the Olympic athlete population through the use of biofeedback and neurofeedback. To address this purpose, two studies were conducted. Study One (Article 1) used a quantitative methodology to explore the relationship between Olympic athletes’ overall self-regulation ability and world ranking. Fifteen Olympic level athletes underwent a 9-stage psychophysiological stress assessment to determine each athlete’s ability to return to baseline after a stress load was applied. Findings revealed that there was a significant correlation between the athletes’ overall self-regulation ability and their ranking at the world level, meaning the better the overall self-regulation ability of the athlete the better the world ranking. Study Two (Articles 2 and 3) employed a qualitative methodology and explored what and how five Olympic level athletes learned from participating in a 20 session biofeedback and neurofeedback training intervention. Data was collected from post-intervention interviews with the athletes. In Study Two, Olympic athletes perceived that the biofeedback and neurofeedback training intervention assisted them in learning to improve self-awareness and self-regulation of their physical and mental states enabling them to feel more in control during sport performances. Engaging in active learning exercises, receiving real-time formative feedback, and utilization of the intervention exercises in training and competition environments were how athletes perceived they learned to self-regulate. Together, the findings from the two studies highlight the relevance and intricacies of self-regulation in high performance sport. Overall, the present dissertation makes a contribution to the sport psychology literature particularly with regard to our understanding of the use of biofeedback and neurofeedback for enhancing self-regulation with Olympic athletes. Thus, learning to improve self-regulation skills using biofeedback and neurofeedback training should be an integral part of a comprehensive and holistic approach used by sport psychology practitioners in assisting athletes to perform to their potential.