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Current clinically available synthetic vascular grafts are made from either polyethylene terephthalate (PET) or expanded polytetrafluoroethylene (ePTFE). In small diameter applications less than 6 mm, these materials are prone to high failure rates caused acutely by blood clot formation and in the mid-term by inflammatory-driven neointimal hyperplasia. A key driver of these modes of graft failure is the slow regeneration of the protective endothelial layer that lines the surface of blood vessels, impaired by the highly hydrophobic polymer surfaces and lack of appropriate biological cues. Surface modifications and presentation of targeted biomolecular cues which promote endothelialisation could address these issues. Identification of the right combination of surface treatment and selection of appropriate cues has proven to be challenging thus far. This thesis explores two different plasma-based modifications of synthetic vascular grafts, to promote rapid endothelialisation. The outcomes of bioengineered grafts were tested under in vitro and in vivo models. Overall, this thesis has demonstrated rapid endothelialisation in two novel synthetic vascular grafts, employing different surface modifications and biomolecules. These findings suggest that both of these approaches have significant potential, justifying further pre-clinical evaluation in the future.