Due to their relatively low cost, large surface area and good chemical and physical properties, carbon nanofibers (CNFs) are attractive for the fabrication of electrodes for supercapacitors (SCs). However, their relatively low electrical conductivity has impeded their practical application. To this end, a novel active-screen plasma activation and deposition technology has been developed to deposit silver, platinum and palladium nanoparticles on activated CNFs surfaces to increase their specific surface area and electrical conductivity, thus improving the specific capacitance. The functionalised CNFs were fully characterised using scanning electron microscope (SEM), energy dispersive X-ray analysis (EDX) and X-ray diffraction (XRD) and their electrochemical properties were evaluated using cyclic voltammetry and electrochemical impedance spectroscopy. The results showed a significant improvement in specific capacitance, as well as electrochemical impedance over the untreated CNFs. The functionalisation of CNFs via environmental-friendly active-screen plasma technology provides a promising future for cost-effective supercapacitors with high power and energy density.