Dynamic equal channel angular pressing (DECAP) and heat treatment are applied to pure Ti to achieve a strength-ductility synergy. DECAP induces a complex multiscale twin structure in Ti including four primary twin types, secondary twins and tertiary twins with multiple variants, and an increased yield strength (58% higher than the as-received Ti). Subsequent annealing at 200 ℃ and 400 ℃ leads to improved ductility and strength. The yield strength (σy) and total elongation (ɛt) for the Ti sample processed with DECAP and 400 ℃ annealing are 555 MPa and 30%, respectively, and its σyɛt product is ∼45% higher than the as-received Ti. DECAP and subsequent annealing lead to a superior strength-ductility synergy in twinned Ti, providing a novel approach to produce high strength and ductility materials via dynamic deformation and subsequent heat treatment.