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Deformed materials usually show a hardening behavior, i.e. enhanced strength accompanied with reduced ductility. Here, we report an extraordinary toughening behavior in cryorolled Zr, i.e. a simultaneous enhancement of the strength and ductility with strain. This unusual increase of ductility results from the motion of preexisting high-density dislocations in tensile processes. The high-density dislocations also contribute to the enhanced strength.