In this work, a novel functionalization strategy for ZIF-67-modified layered MXene was proposed, aiming at improving the fire safety of thermoplastic polyurethanes (TPU). The ZIF-67@MXene was verified by microscopic morphology, elemental composition, functional group species and crystal structure, and then the successfully prepared ZIF-67@MXene was introduced into the TPU material. When ZIF-67@MXene content was only 0.5 wt%, the peak heat release rate, total heat release rate, peak smoke release rate, total smoke release rate, and CO yield of the TPU/ZIF-67@MXene composites were reduced by 26%, 9%, 50%, and 22%, respectively, compared with the pure TPU. The thermogravimetric tests showed that the residual char of TPU/ZIF-67@MXene composites was the most in all samples. In short, the high-quality carbon layer of TPU/ZIF-67@MXene composites acts as a physical barrier to the transfer of heat and toxic gases, greatly improving the flame retardant properties of the TPU polymer.