Spark plasma sintering and hot extrusion processes have been employed for fabricating carbon nanofiber (CNF)-aluminum (Al) matrix bulk materials. The Al powder and the CNFs were mixed in a mixing medium of natural rubber. The CNFs were well dispersed onto the Al particles. After removal of the natural rubber, the Al-CNF mixture powders were highly densified. From the microstructural viewpoint, the composite materials were observed by optical, field-emission scanning electron, and high-resolution transmission electron microscopies. The CNFs were found to be located on every grain boundary and aligned with the extrusion direction of the Al-CNF bulk materials. Some Al carbides (Al4C3) were also observed at the surface of the CNFs. This carbide was created by a reaction between the Al and the disordered CNF. The CNFs and the formation of Al4C3 play an important role in the enhancement of the mechanical properties of the Al-CNF bulk material. The CNFs can also be used for engineering reinforcement of other matrix materials such as ceramics, polymers and more complex matrices.