Pluripotent stem cells (PSCs) represent an exciting cell source for tissue engineering and regenerative medicine due to their self-renewal and differentiation capacities. The majority of current PSC protocols rely on 2D cultures and soluble factors to guide differentiation; however, many other environmental signals are beginning to be explored using biomaterial platforms. Biomaterials offer new opportunities to engineer the stem cell niches and 3D environments for exploring biophysical and immobilized signaling cues to further our control over stem cell fate. Here, we review the biomaterial platforms that have been engineered to control PSC fate. We explore how altering immobilized biochemical cues and biophysical cues such as dimensionality, stiffness, and topography can enhance our control over stem cell fates. Finally, we highlight biomaterial culture systems that assist in the translation of PSC technologies for clinical applications.