A series of waterborne polyurethane (WPU) with different hard segment content were synthesized by a prepolymer mixing process from isophorone diisocyanate, dimethylol propionic acid, the glycolyzed product of poly(ethylene terephthalate) as the soft segment and trimethylol propane as the crosslinking agent. The effect of the hard segment content on the thermal and mechanical properties of WPU films was studied. The results reveal that the hard segment content play a key role in the thermal and physical-mechanical properties of the WPU films. The waterborne polyurethane synthesized from circulating reuse of waste PET materials have good thermal stability and mechanical properties, which is confirmed their potential application as protective and decorative coatings.