Nanostructured metals are usually strong because the ultrahigh density of internal boundaries restricts the mean free path of dislocations. Usually, they are also more brittle because of their diminished work-hardening ability. Nanotwinned materials, with coherent interfaces of mirror symmetry, can overcome this inherent trade-off. We show a bulk nanostructuring method that produces a multiscale, hierarchical twin architecture in a hexagonal closed-packed, solute-free, and coarse-grained titanium (Ti), with a substantial enhancement of tensile strength and ductility. Pure Ti achieved an ultimate tensile strength of almost 2 gigapascals and a true failure strain close to 100% at 77 kelvin. The multiscale twin structures are thermally stable up to 873 kelvin, which is above the critical temperature for many applications in extreme environments. Our results demonstrate a practical route to achieve attractive mechanical properties in Ti without involving exotic and often expensive alloying elements.