Synthesis and comprehensive examination of a polyurethane (urea) elastomer that self-heals based on intrinsic dynamic non-covalent bonds (van der Waals and hydrogen) are reported. The dynamic non-covalent bonds include hydrogen bonds and van der Waals forces. The difference in the previous approach in which hydrogen bond self-healing materials introduced dense quadruple hydrogen bonds at the ends or branched chains poly(propylene carbonate) (PPC) diol was used as the soft segment of the polyurethane (urea) material, and strong van der Waals forces were provided by the large number of carbonyl groups in its main chain; hydrogen bonds were formed by urethane bonds, urea bonds, and the carbonyl groups on PPC. The mechanical properties and healing efficiency of the self-healing polyurethane (urea) elastomer were studied. In situtemperature-dependent infrared and low-field nuclear magnetic resonance (LNMR) measurements were combined with molecular dynamics simulations to investigate the self-healing mechanisms. The results of the studies on the self-healing polyurethane demonstrate that the dynamic cross-linking between hydrogen bonds and van der Waals forces is the basic driving force for the self-healing ability of the material, and temperature is the key factor that affects hydrogen bonding and van der Waals forces. The effect of crystallization on the self-healing ability of the material was also studied. The molecular dynamics simulation results also demonstrate interplay between van der Waals forces and hydrogen bonds at different temperatures.