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For several decades, plasma processing has been employed in the areas of food processing, manufacturing, and agriculture. Plasma processing has also been recognized as greatly beneficial in the field of tissue engineering for the modification of biomaterials. Polyethylene terephthalate (PET) has been employed as a vascular graft material but fails in small diameter applications. In this work, a multifaceted approach combining electrospinning to produce nano- and microscale fibers from PET blended with polybutylene terephthalate (PBT) added for flexibility and plasma modification for enhancing the surface chemistry is demonstrated to be an efficient approach to increase the biocompatibility as evidenced by enhanced fibroblast growth. The analysis of the surface chemistry shows an increase in oxygenated surface functionality, while the bulk analysis shows no significant changes. Thus, an efficient methodology for producing PET/PBT-based grafts that are easily modified with low-temperature plasma and show enhanced biocompatibility for vascular tissue engineering applications is reported.