Cardiovascular disease affects more than 70 million Americans and is the number one cause of mortality in the United States. Because the regenerative capacity of cardiac tissue is limited, human pluripotent stem cells (hPSC) have emerged as a potential source for cellular-based therapies. However, for these therapies to be effective, sufficient amounts of differentiated cells must be produced, these cells must be identified and sorted, and, upon implantation, arrhythmias must be avoided. In this dissertation, I describe the biochemical control of hPSC for their directed differentiation into cardiomyocytes, electrical control for electrophysiology-based cell sorting, and optogenetic control for temporal synchronization. For future therapy, the in vivo application of optical stimulation could allow immediate, precise, and specific synchronization of efficiently derived and purified hPSC-CM with patient cardiac rates and rhythms. This, in turn, would significantly reduce the chance of arrhythmias arising from implanted hPSC-CM, and, therefore, contribute towards establishing a safe and effective cell-based therapy.