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The electrochemical corrosion behaviour of trivalent Cr-C-coated steel samples with Ni and Cu undercoatings was studied in the 0.1 M H2SO4 + 1 g/L NaCl solution. The corrosion resistance of Cr–C-coated samples depends strongly on the undercoating material and the polarised anodic potential. With a soft undercoating, the cracks and crack width in the Cr–C coating can be obviously reduced. Different corrosion potentials were measured from Cr–C-coated steel samples with Ni and Cu-undercoatings. Better electrochemical corrosion resistance of a Cr–C/Cu-coated steel sample was detected at 0 V, but it easily corroded at 0.5 V. On the contrary, the Cr–C/Ni-coated steel sample had better electrochemical corrosion resistance at 0.5 V, and poor at 0 V. The through-coating cracks in the Cr–C coating could provide active corrosion paths for dissolution of the Ni or Cu undercoating during potentiostatic tests polarised at 0 and 0.5 V. The reduction behaviour of Cu2+ ions dissolved from the Cu undercoating of the heat-hardened Cr–C-coated sample was studied and recognised by means of the immersion test in a solution composed of 200 g/L CuSO4·5H2O and 70 g/L H2SO4.