Compared with the traditional polyvinyl butyral (PVB) laminated glass, the polyurethane (PU) based laminated glass has the advantages of higher impact strength and longer service life. Thus, aromatic polyurethane films have attracted more attentions in recent years due to their high light transmittance, adhesion and functionality. In this paper, the tensile strength of polyurethane films based on bis(4âisocyanatocyclohexyl)âmethane (HMDI) have been increased from 27 to 51âMPa and their elongation at break have been increased from 330% to 525% after solvent annealing in toluene. It is attributed to molecular segments with high crystallization and hydrogen bond formation of PU, which are confirmed by FTâIR and XRD characterization. Based on this, laminated glasses with higher impact strength based on the thermoplastic polyurethane films are constructed successfully.