The purpose of this research is to formulate flexible polyurethane elastomers, with different crosslinkers from renewable resources that can be used into cast film materials. Isosorbide moieties were incorporated into the main chains by chain extending the diisocyanate prepolymer which was obtained from polyether diol and hexamethylene diisocyanate. The influence of the crosslinker structure on the polyurethane elastomers was evaluated. The thermal properties of the polymer films were investigated by differential scanning calorimetry and thermogravimetric analysis. These polymers have good thermal stability and increased glass-transition temperatures. The flexible nature of the crosslinkers from renewable resources decreases the rigidity of the elastomers due to of isosorbide moieties. The crosslinked polyurethanes present good mechanical properties with breaking strain in the range of 730–1100% and tensile stress in the range of 5–27MPa. The croslinked samples were thus found to be flexible, eco-friendly materials.