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A Cr₃C₂–NiCr coating with a thickness of 200 μm was deposited on an AISI 1045 steel substrate using a supersonic plasma-spray technique. The hardness of the Cr₃C₂–NiCr coating was characterized by a nano-indenter equipped with an atomic force microscope (AFM). The AFM images indicated that the nano-indents on the Cr₃C₂–NiCr coating exhibited significant “pile-up” deformation. Such pile-up behavior needs to be taken into account in hardness determination because the pile-up height accounts for a large proportion of the indentation depth. In this paper, four different methods are compared to determine the hardness of the Cr₃C₂–NiCr coating: the Oliver–Pharr method, two work-of-indentation methods (total work of indentation and plastic work of indentation), and an AFM analysis method. The results show that the Oliver–Pharr and work-of-indentation methods overestimated the hardness, and the AFM analysis method is considered as a more accurate method for determining the hardness of the Cr₃C₂–NiCr coating.