The mechanical and diffusion properties of Ti-Ta-Fe alloys in the Ti-rich region were investigated by utilizing a high-throughput method, with the combination of nanoindentation and diffusion couple techniques. Five groups of ternary Ti-Ta-Fe diffusion couples were prepared after annealing at 1273 K for 25 h. The composition-dependent mechanical properties of bcc Ti-Ta-Fe system were experimentally determined by means of nanoindentation and electron probe microanalysis (EPMA) techniques. Moreover, the interdiffusion coefficients of Ti-Ta-Fe alloys at 1273 K were confirmed from the composition gradients of the ternary diffusion couples with the support of a pragmatic numerical inverse method. A composition-dependent database on the mechanical and diffusion properties of Ti-Ta-Fe alloys was carefully established and utilized for the discussion of the processability during the hot working. The results indicated that the content of Fe should be controlled for the Ti alloys with high hardness and low Young’s modulus.