A novel kind of damping composite was prepared, which consisted of the tetrapod-shaped ZnO whisker and polyurethane cross-linked epoxy/polyurethane. The dynamic mechanical properties of these materials were investigated by dynamic thermal analysis. Results indicated that the effective damping temperature range (tan δ > 0.3) was obviously broadened from 33.7°C to 178.8°C due to the formation of graft interpenetrating polymer network. With addition of tetrapod-shaped ZnO whisker, the maximal value of damping peak was improved to 1.44 for the increase of the internal friction. The morphological studies proved the existence of partial phase separation, and it was also observed that uniformly dispersed tetrapod-shaped ZnO whiskers were tightly implanted into the polymer matrix. The thermal stability and the tensile strength of composite were improved by the incorporation of tetrapod-shaped ZnO whisker. The results revealed that morphology of graft interpenetrating polymer network and addition of tetrapod-shaped ZnO whisker could provide excellent damping properties for the polymer matrix composite.