Zr was added to Ti-Nb-Fe alloys to develop low elastic modulus and highstrength β-Ti alloysforbiomedical applications. Ingots of Ti-12Nb-2Fe-(2, 4, 6, 8, 10)Zr (at.%) were prepared by arc melting and then subjected to homogenization, cold rolling, and solution treatments. The phases and microstructures of the alloys were analyzed by optical microscopy, X-ray diffraction, and transmission electron microscopy. The mechanical properties were measured by tensile tests. The results indicate that Zr and Fe cause a remarkable solid-solutionstrengthening effect on the alloys; thus, all the alloys show yield and ultimate tensile strengths higher than 510 MPa and 730 MPa, respectively. Zr plays a weak role in the deformation mechanism. Further, twinning occurs in all the deformed alloys and is beneficial to both strength and plasticity. Ti-12Nb-2Fe-(8, 10)Zr alloys with metastable β phases show low elastic modulus, high tensile strength, and good plasticity and are suitable candidate materials for biomedical implants.