Intercalated layered silicates/fluorinated polyimide nanocomposites with good overall properties are synthesized from organics-modified-montmorillonite and poly(amic acid), as confirmed by x-ray and transmission electron microscopy results. Both the bulk and surface (nanometer-domain) mechanical properties of synthesized silicates/fluorinated polyimide nanocomposites increased substantially as compared to that of pure polyimide. In particular, the Young's modulus and surface hardness of the fluorinated polyimide containing 5 wt% 2NH 2-mont are 69% and 100% larger than that of pure polyimide, respectively. Additionally, the reduced elastic modulus by nanoindentation of the nanocomposites is 74% larger than that of the pure polyimide. The barrier properties of the nanocomposites, such as thermal expansion and water absorption retardation, are enhanced.