Materials degradation induced by repeated arc erosion and impact poses a considerable challenge for Ag-based contacts. Fortunately, nature has evolved efficient strategies to construct complex gradient-layered structure that exhibit exceptional erosion and impact resistance. Drawing inspiration by the mantis shrimp appendages, a chain-like CuO nanofibre-reinforced Ag-CuO contact material with a gradient-layered scatter-island/chain-skeleton structure was designed and fabricated. Employing a combined experimental and simulation approach, the evolution of the microstructure during the erosion process was investigated. Results indicated that the interaction between the mantis shrimp appendage-like structure and the chain-like CuO nanofibres effectively suppressed the formation of cracks and pores on the contact surface. Particularly, the scatter-island layer not only played a crucial role in maintaining the viscosity of the molten pool and establishing stable electrical and thermal pathways, but also functioned as a “supplement” to continuously supply a steady source of Ag onto the molten pool surface, effectively promoting CuO skeleton restructuring. Meanwhile, the CuO skeleton diffusive-continuous restructuring of the chain-skeleton layer restricted molten pool flow, significantly enhancing contact erosion resistance. Furthermore, the strong synergistic effect between the gradient-layered structures dispersed stress and deformation concentration on the contact surface. It effectively delayed the defects formation and suppressed interfacial debonding, thereby endowing the contact with excellent impact resistance. Our work presents a fascinated route for designing novel biomimetic Ag-based contacts.