Cardiovascular disorders are a healthcare problem in today's society. The clinically available synthetic vascular grafts are thrombogenic and could induce intimal hyperplasia. Rapid endothelialization and matched mechanical properties are two major requirements to be considered when designing functional vascular grafts. Herein, an electrospun tubular fibrous (eTF) scaffold was biofunctionalized with tropoelastin at the luminal surface. The luminal surface functionalization was confirmed by an increase of the zeta potential and by the insertion of NH2 groups. Tropoelastin was immobilized via its -NH2 or -COOH groups at the activated or aminolysed eTF scaffolds, respectively, to study the effect of exposed functional groups on human endothelial cells (ECs) behavior. Tensile properties demonstrated that functionalized eTF scaffolds presented strength and stiffness within the range of those of native blood vessels. Tropoelastin immobilized on activated eTF scaffolds promoted higher metabolic activity and proliferation of ECs, whereas when immobilized on aminolysed eTF scaffolds, significantly higher protein synthesis was observed. These biofunctional eTF scaffolds are a promising small-diameter vascular graft that promote rapid endothelialization and have compatible mechanical properties.