Stroke is the leading cause of long-term disability with no current treatment addressing post-stroke disability. The complex pathophysiology of stroke and the brain’s limited potential for regeneration prevents sufficient endogenous repair for complete recovery. While engineered materials provide an exciting opportunity to augment endogenous repair in conjunction with other therapies that address post-stroke disability, much of the preclinical work in this arena is still in its infancy. Biomaterials can be used to enhance drug- or stem cell-sustained and targeted delivery. Moreover, materials can act as extracellular matrix-mimics and augment a pro-repair environment by addressing astrogliosis, inflammation, neurogenesis, axonal sprouting, and angiogenesis. Lastly, there is a growing need to elucidate stroke repair mechanisms to identify novel targets to inform material design for brain repair after stroke.