Supercapacitors are energy storage devices with higher energy densities than conventional capacitors but lower than batteries or fuel cells. There is a strong interest in increasing the volumetric and gravimetric capacitance of these devices to meet the growing demands of the electrical and electronic sectors. The capacitance depends largely on the electrode material, and carbon nanofibers (CNFs) have attracted much attention because of their relatively low cost, large surface area, and good electrical conductivity as well as chemical and thermal stability. The deposition of metal nanoparticles on CNFs is a promising way to increase their surface properties and, ultimately, the capacitance of the devices. In this study, nickel and silver nanoparticles were deposited on CNFs using the active screen plasma technology. The CNFs were characterized, and their electrochemical performance was assessed in a three-electrode cell. The results show significant improvements over the untreated CNFs, particularly after functionalization with silver nanoparticles.