The evolutions of phase constitutions and mechanical properties of a β-phase Ti–36Nb–5Zr(wt%) alloy during thermo-mechanical treatment were investigated. The alloy consisted of dual(β t α″) phase and exhibited a double yielding phenomenon in solution treated state. After cold rolling and subsequent annealing at 698 K for 20 min, an excellent combination of high strength(833 MPa) and low modulus(46 GPa) was obtained. The high strength can be attributed to high density of dislocations, nanosized α phase and grain refinement. On the other hand, the low Young’s modulus originates from the suppression of chemical stabilization of β phase during annealing, which guarantees the low β-phase stability. Furthermore, the single-crystal elastic constants of the annealed Ti–36Nb–5Zr alloy were extracted from polycrystalline alloy using an in-situ synchrotron X-ray technique. The results indicated that the low shear modulus C44 contributes to the low Young’s modulus for the Ti–36Nb–5Zr alloy, suggesting that reducing C44 through thermo-mechanical treatment might be an efficient approach to realize low Young’s modulus in β-phase Ti alloys. The results achieved in this study could be helpful to elucidate the origin of low modulus and sheds light on developing novel biomedical Ti alloys with both low modulus and high strength. The evolutions of phase constitutions and mechanical properties of a β-phase Ti-36Nb-5Zr (wt%) alloy during thermo-mechanical treatment were investigated. The alloy consisted of dual (β t α ") phase and exhibited a double yielding phenomenon in After cold rolling and subsequent annealing at 698 K for 20 min, an excellent combination of high strength (833 MPa) and low modulus (46 GPa) was obtained. The high strength can be attributed to high density of dislocations, nanosized α-phase and grain refinement. On the other hand, the low Young’s modulus originates from the suppression of chemical stabilization of β-phase stability. 36Nb-5Zr alloy were extracted from polycrystalline alloy using an in-situ synchrotron X-ray technique. The results indicated that the low shear modulus C44 contributes to the low Young’s modulus for the Ti-36Nb -5Zr alloy, suggesting that reducing C44 through thermo-mechanical treatment might be an efficient approach to realize low Young’s modulus in β-phase Ti alloys. The results achieved in this study could be helpful to elucidate the origin of low modulus and sheds light on developing novel biomedical Ti alloys with both low modulus and high strength.