A new biomedical β-type titanium alloy, Ti-29Nb-13Ta-4.6Zr (TNTZ) has been developed by the authors. Severe plastic deformation (SPD) is a well-proved technique for forming submicron- or nano-sized grain structures in metallic materials. The effect of high-pressure torsion (HPT) processing on the microstructure and the mechanical properties of TNTZ was systematically investigated in this study. TNTZ subjected to HPT processing (TNTZ_<HPT>) shows the nano-sized grains with high-angle grain boundary, which are non-uniform with high dislocation density because of severe deformation. As a result, TNTZ_<HPT> shows a high hardness of around 300 HV and a great tensile strength of around 1050 MPa.