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Two different polymerization methods were used to synthesize the PU/organoclay nanocomposite by either 'one step addition' or 'two step addition' method. In two step addition method, the modified clay was reacted with isocyanate-terminated prepolymer to anchor the polymer chains to the silicate layers before the chain extension reaction occurred. On the other hand, the modified clay and chain extender were added simultaneously in the one step addition method. The effect of polymerization method on the exfoliated/intercalated structure of silicate layers as well as on the microphase separated structure of PU matrix has been studied with FTIR, SAXS and TEM methods. The PU/organoclay nanocomposite prepared with one step addition reaction showed better exfoliated structure which is effectively retarding the micro-phase separation process of PU. However, compared with two step addition one, one step addition method was more effective to enhance the initial modulus and tensile strength of the nanocomposites. The role of modified clay for the segmental orientation process was also studied by infrared dichroism method. The orientation process was hindered by the silicate layers and its effect was more pronounced in the nanocomposite by one step addition method.
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