Polymer nanocomposites containing pristine (PCNF) and aminefunctionalized (NFCNF) electrospun carbon nanofibers were fabricated. The amine-terminated functional groups on CNFs, with a surface coverage of 2.76 mmol/g, react with the epoxy monomers forming covalent linkages for better dispersion and stronger interface. The improved load transfer resulted in an improvement of 82% in storage modulus (rubbery region~70 C) and 20 C increase in the glass transition temperature for 1 wt% NFCNF-epoxy. Tensile strength and modulus improves by 22% and 27%, respectively, for 2 wt % NFCNF-epoxy. The thermal stability, dielectric properties and AC/DC conductivity are discussed in terms of the interfacial characteristics. These results highlight the potential of electrospun CNFs as structural and functional reinforcement.