Ti-based alloys are widely used in biomaterials owing to their excellent biocompatibility. In this study, Ti- Mn-Cu alloys are prepared by high-energy ball milling, magnetic pulsed compaction, and pressureless sintering. The microstructure and microhardness of the Ti-Mn-Cu alloys with variation of the Cu addition and compaction pressure are analyzed. The correlation between the composition, compaction pressure, and density is investigated by measuring the green density and sintered density for samples with different compositions, subjected to various compaction pressures. For all compositions, it is confirmed that the green density increases proportionally as the compaction pressure increases, but the sintered density decreases owing to gas formation from the pyrolysis of TiH2 powders and reduction of oxides on the surface of the starting powders during the sintering process. In addition, an increase in the amount of Cu addition changes the volume fractions of the α-Ti and β-Ti phases, and the microstructure of the alloys with different compositions also changes. It is demonstrated that these changes in the phase volume fraction and microstructure are closely related to the mechanical properties of the Ti-Mn-Cu alloys.