Self-healing polyurethane is a matrix material that can effectively extend the service life of composite materials. The layered two-dimensional Ti 3 C 2 T x material has weak interlayer van der Waals forces, which can undergo slip and form transfer films during friction, reducing shear strength and improving the lubrication performance of the material. Therefore, we introduced two-dimensional Ti 3 C 2 T x into a self-healing polyurethane matrix to improve the lubrication performance of the matrix material. A dual-ion self-healing polyurethane (SPU) was prepared using Nmethyl diethanolamine, hexamethylene diisocyanate, and 1,3propane sultone as raw materials. Ti 3 C 2 T x was prepared by chemical etching, and NH 2 −Ti 3 C 2 T x was obtained by chemically grafting amino groups onto the surface of Ti 3 C 2 T x using aminopropyltriethoxysilane. Then, it was mixed into the SPU matrix to obtain the NH 2 −Ti 3 C 2 T x /SPU composite material. Compared with pure SPU, the friction coefficient and wear rate of the system were reduced by 79.7% and 97.8%, respectively. Under 75%RH and 20 °C conditions, self-healing could be achieved rapidly within 5 min, with a self-healing efficiency of 84.4%. The kind of selflubricating and self-healing polyurethane modified by amination-Ti 3 C 2 T x is expected to be applied in automotive, electronics, and biomedicine.