The organic hybrids of thermoplastic polyurethane (TPU)/hindered phenol (AO-80) were prepared through melt blending, which was followed by hot and cold pressing procedure. The microstructure and dynamic mechanical properties of the hybrids were systematically investigated through SEM, DSC, XRD, FTIR, DMA and a tensile tester. The experimental results indicated that AO-80 was completely dissolved in the matrix. The glass transition of the soft segments of TPU was found to shift to higher temperature with the amount of AO-80 increasing, whereas the glass transition of the hard segments exhibited nearly no evident change, indicating that AO-80 was selectively located in the soft region of TPU and the formation of the strong intermolecular interactions (hydrogen bonding) between AO-80 and the soft region of TPU. With the increase of AO-80 in the hybrids, the tan delta peak gradually shifted to higher temperatures and the maximal tan delta value increased from 0.4 to 1.6. Meanwhile, the glass transition temperature ranges broadened and the TA value increased greatly with the more content of AO-80. Because of the decrease of the hard segments amount in the hybrids, the tensile stress of these hybrids decreased, but still maintained at a high level. The hybrids were expected to have potential applications as high performance damping materials combined with good mechanical properties. (C) 2010 Wiley Periodicals, Inc. J Appl Polym Sci 116:2143-2150, 2010