In this paper, the possibility of improving the damping properties of epoxy resin through dispersion of silicone-intercalated organic montmorillonite was investigated. Flexible silicone macromolecules were inserted into organo-modified montmorillonite (OMMT) by an intercalation to prepare a layered structure that similar to a constrained layer damping structure unit. The effects of silicone macromolecule type, weight ratio of silicone/OMMT and solvent for the intercalation on the structure and properties of the composites were studied by X-ray diffraction (XRD), dynamic mechanical analysis (DMA), and transmission electron microscopy (TEM). The influence of the silicone-intercalated OMMT with different content on the damping properties of the materials was also investigated. The damping property of the final, cured materials was probed using DMA. Analysis of XRD and TEM proved that the silicone-intercalated OMMT had been successfully prepared under an appropriate process. The presence of the silicone-intercalated OMMT decreased the glass transition temperature (Tg) of the epoxy, and the epoxy-nanocomposites achieved a better damping performance.