The mechanical alloying process was used to synthesize the Ni50Al50−xMox nanocrystalline intermetallic compound using pure Ni and Al elemental powder. This process was carried out in the presence of various Mo contents as a micro-alloying element for various milling times. Structural changes of powder particles during mechanical alloying were studied by X-ray diffractometry (XRD) and scanning electron microscopy (SEM). Results showed that mechanical alloying in various combinations was completed after 48 h of milling time. Minimum crystallite size of the as-milled powders (∼10 nm) was achieved after introducing Mo and milling for 128 h. Also, lattice strain decreased with increasing milling time up to 48 h and again increased after 48 h of milling time. On the other hand, the presence of Mo significantly affected variation intensity of the lattice parameter and morphology of the powder particles.