Dicyanate-clay nanocomposite has been prepared by a melt in-situ polymerization method for different modifiers and cation exchange capacity (CEC) values in order to study dispersion and mechanical property. Various dicyanate nanocomposites were prepared by using different MMT systems containing different intercalants which led to different initial gallery heights and packing density. Depending on compatibility between dicyanate and clays, the degree of dispersion varied. Dispersion of clay plates in dicyanate resin depended mainly on CEC and aliphatic chain length of modifier. The lower CEC and shorter aliphatic chain length of modifier gave the exfoliation structure. It was also found that the reactivity of intercalant with dicyanate resin was one of the key factors facilitating the intercalation/exfoliation process of dicyanate/MMT nanocomposites. Shear modulus of reaction-induced dicyanate nanocomposite was significantly increased.