In the present study, mechanical alloying (MA) was employed for synthesising non-equilibrium Zn60Zr40 amorphous powders, and then consolidated into amorphous/crystalline Zn60Zr40 alloys using selective laser melting (SLM). The results showed that the MA process destabilised the atomic periodicity of Zn and Zr powders and induced crystalline-to-amorphous transformation due to atomic size mismatch and negative heat of mixing. Moreover, the amorphisation trend of as-milled powders was intensified with increasing milling time and attained almost fully amorphous structure after 30 h of milling. During SLM, the ultra-high cooling rate restricted the long-range atomic diffusion of the amorphous powders and enabled successful survival of amorphous phase, leading to amorphous/crystalline Zn60Zr40 alloys. The alloys exhibited a maximum compressive yield strength and microhardness of 160.9 ± 9.1 MPa and 3.73 ± 0.8 GPa, respectively. These findings demonstrated that the developed MA-SLM process might be a promising strategy for the preparation of amorphous/crystalline alloys with superior properties.