The allylamine plasma treatment is used to modify the surface properties of vapor grown carbon fibers (VGCF). It is to improve the interfacial bonding between the VGCF and epoxy matrix. The allylamine plasma process was performed by batch process in a vacuum chamber, using gas injection followed by plasma discharge for the durations of 20, 40 and 60 min. The interdependence of mechanical properties on the VGCF contents, treatment time and interfacial bonding between VGCF/ep was investigated. The interfacial bonding between VGCF and epoxy matrix was observed by scanning electron microscopy (SEM) micrographs of nanocomposites fracture surfaces. The changes in the mechanical properties of VGCF/ep, such as the tensile modulus and strength were discussed. The mechanical properties of allylamine plasma treated (AAPT) VGCF/ep were compared with those of raw VGCF/ep. The tensile strength and modulus of allyamine plasma treated VGCF40 (40 min treatment)/ep demonstrated a higher value than those of other samples. The mechanical properties were increased with the allyamine plasma treatment due to the improved adhesion at VGCF/ep interface. The modification of the carbon nanofibers surface was observed by transmission electron microscopy (TEM). SEM micrographs showed an excellent dispersion of VGCF in epoxy matrix by ultrasonic method.