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Exfoliated and intercalated polymer-layered silicate nanocomposites were prepared with enhanced properties. Surface modification of the sodium-montmorillonite was performed with novel ammonium cation containing monomers. Controlled radical polymerization of MMA and styrene was conducted with the help of novel thermal iniferter with or without sodium-montmorillonite. Polyurethane nanocomposites were prepared with different loading of the layered silicates and the properties were compared with the virgin polymers. Structural analysis of the resulting nanocomposites reveals the high degree of penetration of the polymer chains inside the galleries of the layered silicates followed by the uniform exfoliation and intercalation of the layered silicate inside the polymer matrix. DSC and TGA studies reveal the higher glass transition temperature and higher thermal stability of the polymer nanocomposites when compared with the virgin polymers respectively.