The ring opening of γ-valerolactone (GVL) with amine compounds was reported as a promising molecular engineering tool to synthesize precursors for new bio-based polymers such as polyurethanes (PUs). Experimental work on the synthesis of polymers based on GVL/1,2-ethanolamine and GVL/1,2-diaminoethane adducts, and di-isocyanates (1,4-phenylene-di-isocyanate (PDI) 2,4-toluene-di-isocyanate (TDI) and hexamethylene-di-isocyanate (HDI)) is described. The polymers were characterized by FTIR, 1H-NMR, 13C-NMR, elemental analysis and GPC. The best polymerization results were obtained using TEA as the catalyst, DMA as the solvent and a temperature of 140°C for the reaction of the GVL/1,2-aminoethanol adduct with TDI. A polymer with a molecular weight (Mw) of 156 KDalton was produced in 97% yield.