A Ni/C-MoS2 coating was electrospark deposited by using an electrode made of sinered Ni-C-MoS2 composite on a CrNi3MoVA steel substrate, and its nano-mechanical properties and tribological properties were obtained by utilizing nano-indenter and friction-abrasion testing machine. The results showed that the phase constitution of the as-deposited Ni/C-MoS2 coating mainly includes graphite, MoS2, γ-Ni, MoO2, NixS and MoC. Compared with the CrNi3MoVA steel and Ni/MoS2 coating, the Ni/C-MoS2 coating exhibits better tribological properties due to the matrix strengthened by MoO2 and MoC, and the synergistic lubrication effect of graphite and MoS2 in the Ni/C-MoS2 coating.