We added surface-modified silica nanoparticles to poly(ethylene 2,6-naphthalate) (PEN) to investigate their effect on the mechanical properties on the PEN nanocomposite material. The torque and total torque values of the composites decreased in the silica nanoparticle composites. The tensile modulus of the composites reinforced with unmodified silica nanoparticles increased upon increasing the silica content, while the tensile strength and elongation decreased accordingly. In contrast, stearic acid-modified, silica nanoparticle reinforced PEN composites exhibited an increase in elongation and a decrease in tensile modulus upon addition of the silica nanoparticles because the stearic acid that had adsorbed onto the surface of the silica nanoparticle in multilayers could act as a plasticizer during melt compounding. Stearic acid modification had a small effect on the crystallization behavior of the composites. We calculated theoretical values of the tensile modulus using the Einstein, Kerner, and Nielsen equations and compared these values with the experimental data obtained from the composites. The arameters calculated using the Nielsen equation and the Nicolais-Narkis model revealed that the interfacial adhesion between silica nanoparticles and the PEN matrix could be improved.