The transition from a delivery model based on volume to a model based on value is underpinning an unprecedented rate of change in healthcare. Our research identifies academic medical centers that have successfully moved their organizations from a volume-based care delivery model to a model that is based on value, achieving top decile performance in the transition. We asked senior leaders about their key imperatives in achieving system-wide healthcare transformations. Major teaching hospitals were sampled using data envelopment analysis to identify hospitals that produced the best value-based purchasing process of care, Hospital Consumer Assessment of Healthcare Providers and Systems scores, and mortality scores with the most efficient utilization of human and financial organizational resources. On-site interviews were conducted with the CEOs of the top-performing hospitals. Content analysis of the transcribed interviews revealed 10 clear imperatives that our sample of CEOs said were essential.