This research explored the application potential of PUM thin-overlay technology on airport rapid maintenance. The rapid curing process of polyurethane binder determines the limited time window for mixing and construction of polyurethane-bonded mixture (PUM), which presents significant difference with hot-mix asphalt (HMA) technology. Therefore, this research investigated and optimized the mix design of PUM for airport thin-overlay technology based on its thermosetting characteristics. First, limestone and basalt were comprehensively compared as an aggregate for PUM. Then, the effects of molding and curing conditions were studied in terms of mixing time, molding method, molding parameters and curing temperature. Statistical analysis was also conducted to evaluate the effects of gradation and particle size on PUM performances based on gray relational analysis (GRA), thus determining the key particle size to control PUM performances. Finally, the internal structural details of PUM were captured by X-ray CT scan test. The results demonstrated that it only took 12 hours to reach 75% of maximum strength at a curing temperature of 50 °C, indicating an efficient curing process and in turn allowing short traffic delay. The internal structural details of PUM presented distribution of tiny pores with few connective voids, guaranteeing waterproof property and high strength.