This study discusses the interaction model and characterization of a clay organic processed with different swelling agents blended with PU/polymer electrolytes. The change in d-spacing of the clay and modified clay in the PU/polymer electrolytes blends was analyzed using X-rays. A rigid-body pendulum rheometer was used to determine the curing behavior of PU/polymer electrolytes matrix in the clay and modified clay with different proportions. Dynamic mechanical analysis has been applied to discuss the intermolecular interaction between clay and organoclay with different proportions and PU/polymer electrolytes blends. We have also analyzed the mechanical properties, stress, and strain. As a result, the compatibility of polymer electrolytes, clay, and organoclay is better. The swelling agent that intercalated among the layers of clay will be crowded out and adsorbed onto the surface of clay. The curing time, intermolecular interaction, thermal properties, and mechanical properties of composites were clearly influenced by the clay and swelling agent. (c) 2005 Wiley Periodicals, Inc.