In this study, a micro/nano core-shell molybdenum powder was synthesized by mechanochemical process to improve its microstructural uniformity and density by pressureless sintering the core-shell powder. The micro-sized spherical Mo powder, prepared through an electrode induction melting inert gas atomization process, was mixed with MoO3 powder and ball-milled using a three-dimensional shaker mixer. A mechanochemical process involving hydrogen reduction was employed to prepare the core-shell Mo powder. The prepared powders were sintered through the compacting and pressureless sintering. The density was measured using a densitometer to analyze the properties of sintered specimens. Phase analysis was performed using X-ray diffraction. In addition, microstructure analysis was conducted using scanning electron microscopy and electron backscatter diffraction. Comparing the sintered core-shell powder to the sintered conventional mixing powder under the same conditions, we observed that the former exhibited a uniform microstructure and higher density. Furthermore, we experimentally demonstrated the dependence of sintering properties on mixing ratio.