Young's modulus is essential for the design and production of the alloys. Thus, we proposed a MGI (Materials Genome Initiative)-oriented strategy for the high-throughput development of Young's modulus databank in the single-phase alloys. In this study, 17 diffusion couples of the bcc Ti-rich Ti-Nb-Zr, Ti-Nb-Cr and Ti-Nb-Zr-Cr systems annealed at 1273 K for 25 h were experimentally prepared. Subsequently, the composition-dependent Young's moduli and hardness in the bcc Ti-rich Ti-Nb-Zr-Cr system were determined by combining the nanoindentation technique and the electron probe micro analysis (EPMA). Moreover, on the basis of the presently obtained experimental data, the Young's modulus databank in the bcc Ti-Nb-Zr-Cr system were established by means of the CALPHAD (CALculation of PHAse Diagrams) approach. Finally, the Ti-22.6 at.% Nb-30 at.% Zr-3.8 at.% Cr alloy was designed from the Young's modulus databank and verified by using the nanoindentation and cytotoxicity tests. The results reveal that the present MGI-oriented strategy with the combination of the high-throughput measurements and the CALPHAD approach is a very effective method to accelerate the design/development of novel bio-Ti alloys.