This paper gives some insights into the fabrication process of a heterogeneous structured β-metastable type Ti-24Nb-4Zr-8Sn alloy, and the associated mechanical properties optimization of this biocompatible and low elastic modulus material. The powder metallurgy processing route includes both low energy mechanical ball milling (BM) of spherical and pre-alloyed powder particles and their densification by Spark Plasma Sintering (SPS). It results in a heterogeneous microstructure which is composed of a homogeneous 3D network of β coarse grain regions called “core” and α/β dual phase ultra-fine grain regions called “shell.” However, it is possible to significantly modify the microstructural features of the alloy—including α phase and shell volume fractions—by playing with the main fabrication parameters. A focus on the role of the ball milling time is first presented and discussed. Then, the mechanical behavior via shear tests performed on selected microstructures is described and discussed in relation to the microstructure and the probable underlying deformation mechanism(s).