In this paper, nickel coatings (on phosphor bronze substrates) were prepared using pulse electrodeposition method. The friction and wear behaviors of nanocrystalline nickel coating compared with coarse-grained nickel coating against AISI 52100 steel were investigated using l-butyl-3-octylimidazolium tetrafluoroborate ionic liquid and perfluoropolyether as a reference lubricant on reciprocating ball-on-flat UMT-2MT sliding tester. The morphologies of the worn surfaces were observed using a scanning electron microscope. The chemical states of several typical elements on the worn surfaces were examined by means of X-ray photoelectron spectroscopy. The results indicated that NC nickel coatings have better tribological properties than that of coarse-grained nickel coatings under lubricated conditions. This was partly attributed to the high hardness of the NC nickel coating and L-B408 ionic liquid formed tribochemical reaction films under NC nickel coatings.