A previous study showed that Cu can be cold sprayed onto carbon fiber-reinforced polymers (CFRPs) if a Cu interlayer is deposited prior to low-pressure cold spraying. In this present study, Cu was cold sprayed onto CFRP substrates that were coated with either Sn (cold spray) or Ni electroplating. Two layers of Cu powder were also cold sprayed onto a Cu-plated CFRP substrate to investigate the effect of a second particle layer on impacting particles. Test results showed that the relative hardness between the particle and substrate has a major effect on deformability, impact mode, and deposition efficiency (DE), which explains why Cu could not be cold sprayed onto Sn or Ni interlayers and why the deposition efficiency of Cu-on-Cu substrates is lower than that of one pass spraying. In summary, the results suggest that Cu can be successfully cold sprayed at low pressures onto electroplated Cu due to their similarity in hardness.