Poly(vinyl chloride) (PVC)/organophilic-montmorillonite (OMMT) nanocomposites were prepared by direct melt intercalation. PVC/compatibilizer ((vinyl acetate) copolymer (VAc))/OMMT nanocomposites were also prepared by melt intercalation by a masterbatch process. The effect of OMMT content on the nanostructures and properties of nanocomposites was studied. The nanostructures were studied by wide angle X-ray diffraction (WAXD) and transmission electron microscopy (TEM). The linear viscoelastic properties and dynamic mechanical properties of PVC/OMMT nanocomposites were also investigated by an advanced rheometric expansion system (ARES) rheometer. The results showed that partially exfoliated and partially intercalated structures coexisted in the PVC/OMMT and PVC/VAc/OMMT nanocomposites. The mechanical properties test results indicated that the notched Charpy impact strengths of nanocomposites were improved compared to that of pristine PVC and had a maximum value at 1 phr OMMT loadings. The compatibilizer could further improve the impact strengths. But the existence of OMMT decreased the thermal stability of PVC/OMMT and PVC/VAc/OMMT nanocomposites. The linear viscoelastic properties test results indicated the dependence of G and G on shows nonterminal behaviors, and they had better processibility compared with pristine PVC. However, the glass transition temperatures of PVC/OMMT nanocomposites almost had little change compared to that of pristine PVC.