Preparation of pure titanium foil by cold rolling deformation often confronts the strength-ductility trade-off dilemma, how to obtain an excellent strength-ductility combination remains a great challenge. In the present work, we have prepared a pure titanium foil with a bimodal grain (BG) structure consisting of coarse grain (CG) and ultrafine grain (UFG), coupling with high-density deformation twins (DT) via a cryogenic-temperature rolling (CTR) and partial recrystallization annealing (PRA) process. Notably, a high strength-ductility synergy with YS of ∼483 MPa, UTS of ∼517 MPa and elongation of ∼21 % is achieved. The high strength is mainly caused by pronounced fine grain strengthening from the UFG region and twin boundary strengthening from strong interactions between DT and dislocations activated in the CG region. The GND caused by the hetero-deformation between CG and UFG, along with the activation of pyramidal <c+a> dislocation via DT in the CG region endows the pure titanium foil with excellent ductility.
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