A series of polyurethane (PU) composites, which could be used as damping materials, with different contents of hydroxyl silicone oil were successfully prepared in this study. The damping and mechanical properties, thermal stability, and molecular groups of the PU composites were characterized by dynamic mechanical analysis, electronic tensile analysis, thermogravimetric analysis, and Fourier transform infrared (FTIR) spectroscopy, respectively. The surface morphology was also observed via scanning electron microscopy (SEM). FTIR spectroscopy showed that the hydroxyl silicone oil was embedded in the PU. The soft and hard segments of the PU composites appeared thermodynamically incompatible and showed microphase separation, as shown by the SEM pictures. The PU composite with 8% hydroxyl silicone oil was found to possess the best synthetic properties among these composites. The maximum values of tan δ were 0.376, 0.561, and 0.573 at 1, 10, and 20 Hz, respectively. The temperature range for the use of damping materials becomes wider at 1 Hz. Frequencies of 10 and 20 Hz might suitable surroundings for the application of damping materials. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47579.