Mechanical ball milling assisted by sintering in the solid state was used in this research to produce the Zn-Nix system alloy. The derivative powder compositions of Zn-Nix (x = 0, 5, 10, 15, and 20 wt.%) were obtained to study the Ni effects on the microstructural and mechanical properties. It is worth remarking that conventional methods are not appropriate for the manufacture of the Zn-Nix system alloy. The morphological structure and phases were examined by optical microscopy, X-ray diffraction, and SEM/EDS elemental mapping, whereas the mechanical behavior was accomplished by means of a diamond indentation print (Hardness Vickers). The results showed that the intermetallic γ-ZnNi phase did not form during milling time (<4 h); it appears after the sintering process, which is associated with atomic diffusion mechanism through grain boundary at the minimum interfacial energy (ΔG256°C = −13.83 kJ·mol−1). The powder Zn-Ni10 was found to have better properties. Semispherical coarser particles were seen into the metal matrix (Zn δ-hcp structure) as segregates; however, each particle contains an intermetallic compound Zn-Ni that encloses the Ni (α-fcc structure) pure phase. The Ni-α phase was then transformed into a γ-ZnNi intermetallic compound which shifts to higher values of mechanical hardness from about 60 HV to 400 HV units.