Hardness, modulus, and tear strength of PTMEG-based polyurethanes are mainly affected by the hard-segment (MDI/BDO) concentration. On the other hand, PTMEG molecular weight mainly influences low-temperature and dynamic properties. Resilience and hydrolytic stability are affected by both soft-segment concentration and chain length. PTMEG of narrow molecular weight distribution yields softer polyurethanes with considerably longer elongation at break. Broad molecular weight distribution is advantageous only at the lower molecular weight range (650 and 1000), giving rise to improved resilience and low-temperature performance. Polyurethanes made from PTMEG of low molecular weight (Mn≤1000) have inherent drawbacks due to poor phase separation (high Tg) and limits in soft segment concentration (∼63% maximum for PTMEG 1000). The only advantage they offer is easier processability (lower viscosity and melting temperature). On the other hand, PTMEG above 2100 offers little property advantages and is more difficult to handle. Optimum overall polyurethane properties can be achieved with PTMEG in the molecular weight range of 1800 to 2100. It is conceivable that PTMEG-based polyurethanes made with different diisocyanates, curatives, curative/NCO ratios, or in the presence of triols or catalysts may show similar trends as the MDI/BDO formulations described in this study.