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In this work, a series of binary Ti–Mo alloys with the Mo contents ranging from 3.2 to 12 at.% were prepared using non-consumable arc melting. The microstructures were investigated by X-ray diffraction and transmission electron microscope, and the elastic modulus was evaluated by nanoindentation testing technique. The evolution of the volume fractions of ω phase was investigated using X-ray photoelectron spectroscopy. The results indicated that the phase constitution and elastic modulus of the Ti–Mo alloys are sensitive to the Mo content. Ti–3.2Mo and Ti–8Mo alloys containing only α and β phases, respectively, have a low elastic modulus. In contrast, Ti–4.5Mo, Ti–6Mo, Ti–7Mo alloys, with different contents of ω phase, have a high elastic modulus. A simple micromechanical model was used to calculate the elastic modulus of ω phase ( E ω ), which was determined to be 174.354 GPa.