Cardiovascular diseases (CVD) such as ischemic heart disease and peripheral artery disease, continue to be the leading cause of death worldwide. The primary underlying cause of these diseases is atherosclerosis, the deposition of cholesterol, lipids, and calcium leading to plaque formation within the blood vessel wall, causing thickening and hardening of the tissue and obstruction of blood flow. Implantable medical devices, including vascular grafts and stents, can be used to reintroduce blood flow downstream of the obstructed area. The current gold standard for surgical intervention in CVD is the use of autologous vessels to bypass the obstructed flow. However, patients often lack suitable vessels requiring the use of synthetic graft materials. This dissertation describes novel biomaterials and therapeutics designed for vascular applications for the advancement of cardiovascular medicine.