Polyurethane elastomers of a controlled molecular architecture were synthesized using a two-step polymerization technique. The building blocks of the elastomeric materials included urea-urethane prepolymers end-capped with diisocyanate groups and had an exact number of urea groups at both ends. Two-dimensional bifurcated hydrogen-bonding networks incorporating the urea groups were, with differential scanning calorimetric and dynamic mechanical thermal analyzer techniques, responsible for the increase in the glass-transition temperature (T-g) of the hard block and sharp interface morphology between the pure "hard" domains and pure "soft" domains. The higher extent of the phase separation between the two phases contributed to higher elastic moduli for the hard blocks and higher tensile strength for the elastomeric samples. Higher elongation values were attributed to the liberation of the elastomeric chain ends that otherwise would have been constrained in the interface region. The higher T-g values of the hard blocks corresponded to an increase in the hardness values and a decrease in the tear-strength values. The increase in the amount of urea groups within the hard segments, as a result of the increased amount of water and blowing catalyst, resulted in elastomeric foams with higher open-cell content. This resulted in lower resilience values as measured using the pendulum rebound test and was attributed to the ability of the open cells to absorb and dissipate energy.