Titanium β-type alloys are preferred biomaterials for hard tissue replacements due to the low Young modulus and limitation of harmful aluminum and vanadium present in the commercially available Ti6Al4V alloy. The aim of this study was to develop a new ternary Ti-Zr-Nb system at 36≤Ti≤70 (at. %). The technical viability of preparing Ti-Zr-Nb alloys by high-energy ball-milling in a SPEX 8000 mill has been studied. These materials were prepared by the combination of mechanical alloying and powder metallurgy approach with cold powder compaction and sintering. Changes in the crystal structure as a function of the milling time were investigated using X-ray diffraction. Our study has shown that mechanical alloying supported by cold pressing and sintering at the temperature below α→β transus (600°C) can be applied to synthesize single-phase, ultrafine-grained, bulk Ti(β)-type Ti30Zr17Nb, Ti23Zr25Nb, Ti30Zr26Nb, Ti22Zr34Nb, and Ti30Zr34Nb alloys. Alloys with lower content of Zr and Nb need higher sintering temperatures to have them fully recrystallized. The properties of developed materials are also engrossing in terms of their biomedical use with Young modulus significantly lower than that of pure titanium.