The epoxidized hydroxyl-terminated polybutadiene (EHTPB) with different epoxide number was prepared by peroxide acetic acid in situ. EHTPB based polyurethane was prepared by curing with diisocyanates (toluene-diisocyanate（TDI）, isophorone-diisocyanate(IPDI) and 4,4-dicyclohexylmethane-diisocyanate(H₁₂MDI), and chain extender 1,4-butanediol(BDO)). Its structure was also analyzed by infrared spectroscopy and scanning electron microscopy (SEM). Results show that H₁₂MDI is a better solidified agent for improving mechanical properties of polyurethane. The optimal epoxide number of EHTPB is about 0.18 mol·(100 g)^-1. Mechanical properties of polyurethane can be improved by adding extender BDO. The optimal content of BDO is that the mole ratio of —OH(BDO) /—OH(EHTPB) is 1-2. The experimental results indicate that EHTPB/H₁₂MDI/BDO based polyurethane has the highest mechanical properties.