To create a library of alloy compositions for high-throughput combinatorial evaluation using correlative optical and electron microscopy with EBSD and nanoindentation, a block with a compositional gradient of molybdenum from 2 weight percent to 10 weight percent in titanium was constructed in the current study using the direct energy deposition technique for metal additive manufacturing. A basketweave microstructure with varying alpha lath size, number density, and alpha-beta phase percentage was found throughout the sample by microstructural examination. The rise in Mo content, which functions as a beta stabiliser, caused the beta phase fraction to evolve from 12% at the bottom to 57% at the top, according to the EBSD data. Furthermore, the findings of the EDS mapping indicated a higher solute concentration along the boundaries of the alpha laths. However, the elastic modulus increased from 124±3 GPa to 127±2 GPa before falling to 106±5 GPa at the top. A similar trend was also seen in the hardness results, which showed an increase in hardness from 4±0.2 to 9±0.5 GPa at the bottom and a decrease to 1.4±0.2 GPa at the top. This trend in elastic modulus and hardness may be explained by the development of martensitic phases (α’, α”, ω) and strengthening of solid solutions at lower Mo concentrations, whilst the decline in hardness may be explained by the dominance of the softer beta phase at higher Mo concentrations. The findings of the texture analysis supported the presence of Burger's orientation relationship: {0002}α || {110}β and <112 ̅0>α || <1 ̅10>β throughout the sample with fewer variants present at the top indicating variant selection becoming stronger from the bottom to the top of the sample. Moreover, parent beta grains were reconstructed which shows a coarser grain morphology. In addition, nano-indentation studies were used to determine elasto-plastic response of different microstructures to establish processing – composition – microstructure - mechanical property for a large Ti-Mo alloy library for preliminary alloy screening for different applications.