To regulate the rapid reaction kinetics of 3,3’-dichloro-4,4’-diaminodiphenylmethane (MOCA) chain extension in cast polyurethane (CPU) elastomers, a solvent casting strategy was developed. By dissolving MOCA in ethyl acetate, the pot life was significantly extended from <20 s to >10 min, enabling homogeneous mixing and processing. A series of CPUs were synthesized using polytetrahydrofuran ether glycol (PTMEG-1000) as the soft segment and different diisocyanates (TDI and MDI-50) as the hard segment monomers. The hard segment content exerted a significant influence on the mechanical properties, with an nTDI: nPTMEG ratio of 2: 1 yielding an optimal tensile strength of 50.74 MPa. Furthermore, the hard segment composition played a critical role: MDI-50-based CPUs exhibited superior thermal stability. Blending TDI with MDI-50 allowed for tunable properties, and a molar ratio of nMDI: nTDI = 5: 5 resulted in the poorest mechanical properties (35.96 MPa). This work provides a practical and effective approach to tailoring the comprehensive properties of high-performance CPU elastomers for demanding applications.