Carbon nanofilament and nanotubes (CNTs) have shown promise for enhancing the mechanical properties of fiber-reinforced composites (FRPs) and imparting multi-functionalities to them. While direct mixing of carbon nanofilaments with the polymer matrix in FRPs has several drawbacks, a high volume of uniform nanofilaments can be directly grown on fiber surfaces prior to composite fabrication. This study demonstrates the ability to create carbon nanofilaments on the surface of carbon fibers employing a synthesis method, graphitic structures by design (GSD), in which carbon structures are grown from fuel mixtures using nickel particles as the catalyst. The synthesis technique is proven feasible to grow nanofilament structures—from ethylene mixtures at 550 °C—on commercial polyacrylonitrile (PAN)-based carbon fibers. Raman spectroscopy and electron microscopy were employed to characterize the surface-grown carbon species. For comparison purposes, a catalytic chemical vapor deposition (CCVD) technique was also utilized to grow multiwall CNTs (MWCNTs) on carbon fiber yarns. The mechanical characterization showed that composites using the GSD-grown carbon nanofilaments outperform those using the CCVD-grown CNTs in terms of stiffness and tensile strength. The results suggest that further optimization of the GSD growth time, patterning and thermal shield coating of the carbon fibers is required to fully materialize the potential benefits of the GSD technique.Published version