The microstructure and mechanical properties of polypropylene (PP)/OMMT binary nanocomposites and PP/styrene-6-(ethylene-co-butylenes)-6-styrene triblock copolymer (SEBS)/OMMT ternary nanocomposites were investigated using X-ray diffraction (XRD), transmission electron microscopy (TEM), and rheology and electromechanical testing machine. The results show that the organoclay layers are mainly intercalated and partially exfoliated in the PP-based nanocomposites. The additions of SEBS and OMMT have no significant effect on the crystallization behavior of PP. At the same time, it can be concluded that the polymer chains of PP and SEBS have intercalated into the organoclay layers and increase the gallery distance after blending process based on the analytical results from TEM, XRD, and rheology, which result in the form of a percolated nanostructure in the PP-based nanocomposites. The results of mechanical properties show that SEBS filler greatly improve the notched impact strength of PP, but with the sacrifice of strength and stiffness. OMMT can improve the strength and stiffness of PP and slightly enhance the notched impact strength of PP/ PP-g-MA. In comparison with neat PP, PP/OMMT, and PP/SEBS binary composites, notched impact toughness of the PP/SEBS/OMMT ternary composites significantly increase. Moreover, the stiffness and strength of PP/ SEBS/OMMT ternary nanocomposites are slightly enhanced when compared with neat PP. It is believed that the synergistic effect of both SEBS elastomer and OMMT nanoparticles account for the balanced mechanical performance of the ternary nanocomposites.