The overall process, from the pre-treatment of aluminum substrates to the eco-friendly neutral electroless Ni-P plating process, was observed, compared, and analysed. To remove the surface oxide layer on the aluminum substrate and aid Ni-P plating, a zincation process was carried out. After the second zincation treatment, it was confirmed that a mostly uniform Zn layer was formed and the surface oxide of aluminum was also removed. The Ni-P electroless plating films were formed on the secondary zincated aluminum substrate using electroless plating solutions of pH 4.5 and neutral pH 7.0, respectively, while changing the plating bath temperature. When a neutral pH7.0 electroless solution was used, the Ni-P plating layer was uniformly formed even at the plating bath temperature of 50 oC, and the plating speed was remarkably increased as the bath temperature was increased. On the other hand, when a pH 4.5 Ni-P electroless solution was used, a Ni-P plating film was not formed at a plating bath temperature of 50 oC, and the plating speed was very slow compared to pH 7.0, although plating speed increased with increasing bath temperature. In the P contents, the P concentration of the neutral pH 7.0 Ni-P electroless plating layer was reduced by ~ 42.3 % compared to pH 4.5. Structurally, all of the Ni-P electroless plating layers formed in the pH 4.5 solution and the neutral (pH 7.0) solution had an amorphous crystal structure, as a Ni-P compound, regardless of the plating bath temperature.