This work intends to produce smart materials for use in advanced applications such as artificial load resisting tissues and articular implants by exploiting the good strength of carbon nanofibers (CNFs) and the excellent biocompatibility of polydimethylsiloxane (PDMS). In this work, a series of CNF/PDMS nanocomposites was fabricated by varying the method of preparation and nanofiber surface modification. Dynamic mechanical properties and creep behavior of these hybrid materials were studied in order to comprehend the reinforcing effect of the nanofibers on the polymer matrix. The improvement was overwhelming with 74% enhancement in storage modulus and 1100% reduction in creep compliance for just 4 phr of amine modified CNF. Property improvement in the nanocomposites is a function of the extent of nanofiber dispersion in the polymer matrix which was examined by High Resolution Transmission Electron Microscopy (HRTEM) and Field Emission Scanning Electron Microscopy (FESEM).