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In the case of electrical contact, copper alloys are often unable to withstand arc ablation and premature failure. To solve this issue, Ni-8wt.%Al (Ni–8Al) coatings were successfully prepared on copper substrates utilizing the high-speed laser cladding. In addition, the microstructure evolution, microhardness, electric conductivity and arc ablation resistance of the prepared coatings were investigated in detail. As a result, the achieved Ni–8Al coatings were structurally dense with good metallurgical bonding to the substrate, of which the microstructure showed a bottom-up evolution of fine sub-grain structure. Notably, the microhardness of the coating was 191.7 HV0.2, representing an increase of 82.57% compared to the substrate, and the electrical conductivity was 18.03 %IACS, approaching that of pure nickel. Additionally, the increase in ablation currents led to changes in the ablation behaviors and failure mechanisms of both the substrate and coating. At high currents, a huge arc ablation crater appeared in the center of the substrate due to the reaction force of the anode flame and the difference in surface tension between the liquid metal at the center and the edge of the molten pool. Nevertheless, the coatings showed better arc ablation resistance due to the improvement of molten pool stability during arc ablation by the in situ formed Al2O3 layer on the coating surface.