The effects of atmospheric plasma treatment and matrix modification by maleic anhydride PP (MAPP) addition, respectively, on the mechanical properties of vapor grown carbon fiber (VGCF)/polypropylene (PP) were investigated. Raw VGCF/PP, raw VGCF/MAPP, atmospheric plasma-treated (APT) VGCF/PP were melt mixed and extruded using a twin-screw extruder. The tensile modulus, shear modulus, and shear strength of APT VGCF/PP showed higher values than those of raw VGCF/PP. The tensile strength, flexural modulus, and flexural strength of raw VGCF/MAPP demonstrated higher values than all the other samples of raw VGCF/PP. The mechanical properties were improved with the atmospheric plasma treatment and coupling agent due to the improved adhesion at VGCF/PP interface. SEM micrographs revealed an excellent dispersion of VGCF in PP and MAPP, respectively. From the twin-screw extruder processing, the VGCF particles were relatively well aligned as well.