Engineered polymer nanofibers are materials with high potential to form composite materials. Electrospinning is a technique that allows preparation of such fibers with a high degree of nanometric scale control. This study explores the preparation of polymer nanocomposites reinforced with nylon nanofibers through impregnation. The polymer matrix consists of water soluble polymers, and engineering polymers for structure and electronic applications such as polyvinylidine pyrrolidone, PP and poly-dimethyl siloxane, respectively. The procedure involves deposition of the electrospun nylon nanofibers on a substrate. Fiber orientation and morphology were studied using scanning electron microscopy and small-angle light scattering, and mechanical properties were studied under uniaxial tensile deformation. The results showed that preparation of nanocomposites using nylon nanofibers is feasible, and the nanofibers significantly improved the mechanical properties of the polymer matrix.