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In order to improve the buffering performance of a walkable lunar lander (WLL), an optimization method of multi-layer combined gradient cellular structure (MCGCS) is proposed. The impact load, impact action time, impact overload, and deformation amount are analyzed. The buffering performance of the material is evaluated and verified effectively with the simulation data. The overload acceleration of the WLL, the volume, and mass of the buffer material were set as the space-time solution to the optimal buffer problem, and the complex relationship between the material structure parameters and the buffer energy absorption (EA) parameters was established based on the sensitivity analysis method, and the buffer structure parameters were automatically optimized. The buffer energy absorption characteristics of the MCGCS are like the simulation results, and it has a good buffering effect, which provides a new research perspective for the excellent landing buffering mechanical properties of the WLL and a new idea for the application of engineering materials.