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The potential application of carbon nanoparticles such as carbon nanotubes (CNT), carbon nanofibers (CNF) and graphene (G) flakes grown on carbon fiber (CF) surface as fillers in polypropylene composite is discussed. Carbon fiber surface must be modified before it can be used as fillers in composites. A one-step process using the chemical vapor deposition (CVD) method has been used to synthesize CNT, CNF and G and also G-CNF and G-CNT on the carbon fiber to modify its surfaces. In this study, CFs (Toho Tenax Co. Ltd.) was utilized as a substrate to grow carbon nanostructures and also as a filler in polypropylene pellets (PP 600G) polymer matrix. To the best of our knowledge, so far nobody has reported any work being widely carried out on synthesizing G layers on the CNF and CNT grown on CF by using a bimetallic catalyst (Ni/Cu) in a one-step CVD method in order to increase the CF surface area as well as to improve its properties.