In this work, a novel strategy is developed to solve the issue of mutually exclusive high mechanical robustness and thermo-stability for thermoplastic polyurethane (PU). A leaf-like and reticulate interfingering superstructure can be seen. The superstructure of polyurethanes can also be tuned by the polarity of chain extender molecular via changing the number for ferrocene redox centres, thus to further enhance the thermal stability and elasticity of PUs. As a result, by incorporating bisferrocene units into the main chain of PU, a high-performance PU elastomer can be synthesized with a highest initial degradation temperature of T 5% of 345 °C, a highest tensile strength of 42.3 MPa with an elongation over 1000%, as well as a toughness of 19.6 GJ m-3. These results conclusively suggest that high-performance thermoplastic polyurethane elastomers had great promise for potential application in a wide range of practical fields.
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