Mechanical ball milling assisted by sintering in the solid state was used in this research to produce the Zn-Ni x system alloy. e derivative powder compositions of Zn-Ni x (x 0, 5, 10, 15, and 20 wt.%) were obtained to study the Ni e ects on the microstructural and mechanical properties. It is worth remarking that conventional methods are not appropriate for the manufacture of the Zn-Ni x system alloy. e morphological structure and phases were examined by optical microscopy, X-ray di raction, and SEM/EDS elemental mapping, whereas the mechanical behavior was accomplished by means of a diamond indentation print (Hardness Vickers). e 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 di usion mechanism through grain boundary at the minimum interfacial energy (ΔG256°C −13.83 kJ·mol
−1).e powder Zn-Ni 10 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.e 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.