It is still a challenge to prepare high performance rubber/MMT composites by one‐pot method without solution. In this work, NBR/AO60/montmorillonite (MMT) (NBR/AM) composites were prepared by mechanical blending method and in‐situ formation of surface hydrogen bond was introduced under vulcanization process. Results showed that the polar parts of melting AO60 could partly intercalate into interlayer of MMT and some parts of melting AO60 molecules were absorbed onto surfaces of MMT particles during the vulcanization process. Subsequently, surface hydrogen bonds were constructed among NBR, AO60, and MMT after natural cooling, as evidenced by FTIR, resulting in more complex morphology and good interfacial adhesion in the NBR/AM composite. Consequently, as compared to NBR/montmorillonite (NBR/M) composite, remarkable improvements were found in mechanical properties and energy dissipation at high temperature of NBR/AM composite, which may provide a new prospect for designing high performance damping materials.
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