Composite materials with nanofibrous reinforcements are capable of high mechanical performance and enhanced properties despite their low volume fraction of reinforcement. In this study, tensile properties of epoxy-matrix nanocomposites were investigated after reinforcing by hand layup method implementation of randomly oriented electrospun nanofiber layers. The reinforcements were produced from polyacrylonitrile (PAN), Polyamide-6,6 (PA-6,6), and their 50/50 hybrid. The results indicated that PAN enhanced the tensile toughness of the matrix by almost 4 times, increasing both the ductility (an expected 23% due to fiber being more elastic than the matrix) and the ultimate tensile strength (a surprising 35% even though the fibers were less stiff than the matrix). These results indicate significant improvements in the impact properties for advanced applications. The results revealed that PA-6,6 did not show the characteristics of a promising reinforcement whether used solely or added to PAN.