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Polyurethane (PU) materials with high strength, toughness, anti‐wear properties, and high heat resistance are in high demand for dynamic sealing applications. In this study, a series of high‐performance crosslinking polyurethanes (CPUs) were prepared by pre‐polymerization of polycarbonate diol (PCDL) with toluene‐2,4‐diisocyanate (TDI), followed by crosslinking with trimethylolpropane (TMP). The molar ratio (R) of PCDL/ TDI and the degree of cross‐linking were found to significantly affect the microphase separation. The results indicate that as the R‐value increases, the transition temperature of CPUs increases from 6.0°C to 82.4°C, and the tensile strength increases from 21.1 ± 2.5 MPa to 46.0 ± 3.6 MPa. Moreover, the CPUs exhibit excellent heat resistance (with a heat resistance index of ~150°C) and hydrolysis resistance, attributed to the high crystallinity of PCDL and the synergistic effect of chemical crosslinking. Additionally, the CPUs demonstrate low friction coefficient (COF = 0.01–0.062), exceptional anti‐wear properties (Akron wear, 0.11–0.07 cm3/1.61 km), and outstanding fatigue resistance. These desirable characteristics make CPUs suitable for use as dynamic sealing or lubricating materials in harsh conditions, thereby extending the service life of seals and preventing leakage and other related issues. [ABSTRACT FROM AUTHOR]