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Polyurethane (PU) plays a critical role in elastomers, adhesives, and self-healing materials. We selected the most commonly used aromatic isocyanates, 4,4′-methylene diphenyl diisocyanate (MDI) and tolylene-2,4-diisocyanate (TDI), and the most commonly used aliphatic isocyanates, hexamethylene diisocyanate (HDI), isophorone diisocyanate (IPDI), and dicyclohexylmethane-4,4′-diisocyanate (HMDI), as raw materials, combined with polytetramethylene ether glycol (PTMG) and 1,4-butanediol (BDO) to successfully synthesize five PU materials. The effects of isocyanate structure on polymerization rate, hydrogen bonding, thermal properties, phase separation, wettability, self-healing performance, adhesion, and mechanical properties were systematically investigated. The results show that isocyanates with higher symmetry facilitate hydrogen bonding, but excessive flexibility and crystallinity may inhibit its formation. MDI-based PU exhibits the highest hydrogen bonding index (HBI) of 4.10, along with the most distinct phase separation and the highest tensile strength of 23.4 MPa. HMDI-based PU demonstrates the best adhesion properties, with the highest lap shear strength of 7.9 MPa, and also exhibits excellent scratch healing ability. IPDI-based PU shows good self-healing performance, recovering 88.7% of its original tensile strength and 90.6% of its original lap shear strength after heating at 80 °C for 24 h. Furthermore, all the samples can be reprocessed by melt or solution methods, showing excellent recyclability. [ABSTRACT FROM AUTHOR]