By employing the melt blending method, selective hindered amines were oriented to disperse in the hard phase of thermoplastic polyurethane (TPU). The microstructure and performance of organic hybrids consisting of TPU and poly-[(1-hydroxyethyl -2,2,6,6- tetramethyl-4-hydroxyl piperidine)]-glycolsuccinate (GW-622) and poly{[6-(1,1,3,3-tetramethylbutyl) -imino]-[1,3,5-triazine-2,4- dimethyl] 1242,2,6,6- tetramethyl piperidinyl)- imino]-cyclohexane-[4-(2,2,6,6-tetramethyl piperidinyl)-imino]} (GW-944) were investigated by dynamic mechanical analysis (DMA), differential scanning calorimetry (DSC), scanning electric microscopy (SEM), and tensile measurement. The neat TPU matrix displayed only one glass transition peak in the DMA curve, whereas the TPU/GW-622 hybrids exhibited two overlapping loss peaks, and the TPU/GW-944 hybrids demonstrated two separated relaxation peaks. The second excited relaxation peak of the hybrids was attributed to the oriented distribution of hindered amine in TPU and strong intermolecular interactions between the hindered amine and the hard segments of TPU. The complex and interesting evolution in structure and properties of the hybrids with hindered amine incorporation was interpreted. The loss peak areas (TA) of the hybrids increased greatly, and the high temperature damping properties was expected to improve. This kind of novel hybrid presented a promising future as high performance damping material. (C) 2010 Wiley Periodicals, Inc. J Appl Polym Sci 120: 906-913, 2011