A hybrid functional nanomaterial was synthesized by functionalizing carbon nanofibers (CNF) with polyhedral oligomeric silsesquioxane (POSS). The reaction between CNF and the amine group of ocataminophenyl POSS was achieved using carbodiimide chemistry. The CNF-POSS hybrids were designed to increase the reactivity of CNF without affecting its inherent properties. The reactive amine groups of CNF-POSS were further modified with an oligomer of polyimide polymer to improve the interaction with the polymer matrix, thus forming a nanocomposite with enhanced multifunctional properties. Functionalization was characterized using thermal gravimetric analysis (TGA), x-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM).