Mo-Cu alloys have been widely used for heat sink materials, vacuum technology, automobile, and many other applications due to their excellent physical and electric properties. Especially, Mo-Cu composites with 5 ~ 20 wt.% copper are widely used for the heavy duty service contacts due to their excellent properties like low coefficient of thermal expansion, wear resistance, high temperature strength, and prominent electrical and thermal conductivity. In most of the applications, highly-dense Mo-Cu materials with homogeneous microstructure are required for better performance. In this study, Mo-Cu alloys were prepared by PBM (planetary ball milling) and SPS (spark plasma sintering). The effect of Cu with contents of 5~20 wt.% on the microstructure and thermal properties of Mo-Cu alloys was investigated.