A simple and low-cost electroless deposition technique is used to prepare nickel-doped carbon nanotubes under different doping conditions, and to explore the influence of different nickel doped samples on the electrical contact properties of carbon nanotubes. First, the original carbon nanotubes are subjected to mixed acid oxidation, sensitization and activation treatment. Subsequently, the nickel chloride hexahydrate is used as the main salt and dimethylamine borane is used as the reducing agent to prepare the electroless deposition solution. And then, the prepared carbon nanotube dispersion is dropped into the electroless deposition solution to obtain the sample of nickel-doped carbon nanotubes. Morphological characterization indicates that the nanoparticles with different particle sizes and doping amounts could be doped on the surface of carbon nanotubes under different deposition conditions. The X-ray energy spectrum shows that the main component of the doped nanoparticles is nickel, and the further X-ray photoelectron spectroscopy reveals the constituent valence state of nickel. However, the Raman spectra indicate that the doping type of nickel-doped carbon nanotubes by this deposition method is the P-type. Finally, the electrical contact performance test results show that the electrical contact properties between gold electrodes and nickel-doped carbon nanotubes with different particle sizes and doping contents are different, but that all of them can be improved to a certain extent. According to the order of nanoparticles with a small particle size and a moderate amount, those with a moderate particle size and a moderate amount, and those with a large particle size and a large amount in the nickel-doped sample, the average value of the contact resistance decreases by 32.70%, 71.63% and 49.33%, respectively.