Polymeric and metallic materials are used extensively in permanently implanted cardiovascular devices and devices that make temporary but often prolonged contact with body fluids and tissues. Foreign body responses are typically triggered by host interactions at the implant surface, making surface modifications to increase biointegration desirable. Plasma-based treatments are extensively used to modify diverse substrates; modulating surface chemistry, wettability and surface roughness, as well as facilitating covalent biomolecule binding. Each aspect impacts on facets of vascular compatibility including endothelialization and blood contact. These modifications can be readily applied to polymers such as Dacron and expanded polytetrafluoroethylene, which are widely used in bypass grafting and the metallic substrates of stents, valves and pacemaker components. Plasma modification of metals is more challenging given the need for coating deposition in addition to surface activation, adding the necessity for robust interface adhesion. This review examines the evolving plasma treatment technology facilitating the biofunctionalization of polymeric and metallic implantable cardiovascular materials.