One of the most important requirements for a metallic biomaterial is the mechanical biocompatibility, which means excellent mechanical properties—high strength and fatigue strength, but low elastic modulus, to be mechanically harmonized with hard tissues. In order to improve the mechanical and biocompatible performance of the Ti-25.5Nb-4.5Ta-8.0Zr wt% alloy, the influence of cold plastic deformation and solution treatment on its properties were investigated. The Ti-25.5Nb-4.5Ta-8.0Zr wt% alloy was fabricated by melting in a cold crucible furnace (in levitation) and then subjected to several treatment schemes, which include cold rolling and different solution treatments. Microstructural and mechanical characteristics of specimens in as-cast and thermo-mechanically processed condition were determined by SEM microscopy and tensile testing, for different structural states: initial as-cast/as-received, cold rolled and solution treated at different temperatures (800, 900, and 1000 °C) and durations (5, 10, 15, and 20 min), with water quenching. It was concluded that both cold rolling and solution treatment have important positive effects on structural and mechanical properties of the biomaterial, increasing mechanical strength and decreasing the elastic modulus. Samples in different structural states were also corrosion tested and the results provided important information on determining the optimal processing scheme to obtain a high-performance biomaterial. The final processing route chosen consists of a cold rolling deformation with a total deformation degree of 60%, followed by a solution heat treatment at 900 °C with maintenance duration of 5 min and water quenching. By applying this thermo-mechanical processing scheme, the Ti-25.5Nb-4.5Ta-8.0Zr wt% alloy showed an elastic modulus of 56 GPa (5% higher than in the as-cast state), an ultimate tensile strength of 1004 MPa (41.8% higher than in the as-cast state), a yield strength of 718 MPa (40.6% higher than in the as-cast state), and increased corrosion resistance (the corrosion rate decreased by 50% compared to the as-cast state).