Intercalated or exfoliated nanocomposites were composed by the novolac cured epoxy and one of three different kinds of layered silicates, such as montmorillonite (PK-802), saponite (Semecton-SA) and nontronite (PK-805). The bi-functional modifiers (PI/BEN or MI/BEN) with different ratio, which contained one of the promoters (2-phenylimidazole, PI and 2-methylimidazole, MI) of epoxy and benzalkonium chloride (BEN), were intercalated into the gallery regions of pure clays at the same time and followed by a crosslinking reaction. The properties of novolac cured epoxy/clay nanocomposites were characterized by wild-angle X-ray diffraction (WAXRD), thermal analysis (TGA/DSC), coefficiency of thermal expansion (TMA), mechanical properties (DMA), and transmission electron microscopy (TEM). According to the measurement, these novolac cured epoxy-clay nanocomposites have shown the significant improvement in the thermal, mechanical and barrier properties.