Gradient nanostructure was introduced to enhance the strength and ductility via deformation incompatibility accommodated by geometrical necessary dislocations for most metallic materials recently. However, few intensive researches were carried out to investigate the effect of gradient structure on the deformation twin evolution and resulting performance improvements. In the present paper, we produced gradient-structured AZ31 Mg alloy with fine-grain layers, parallel twin laminates and a coarse-grain core from two upmost surfaces to the center of plate. Surprisingly, this architected Mg alloy exhibited simultaneous enhancement of strength and ductility. Subsequent microstructural observations demonstrated that abundant twin-twin interactions resulting from higher strength and multi-axial stress state could make great contributions to the increase of work-hardening capability. This was further proved by the measurement of full-field strain evolution during the plastic deformation. Such a design strategy may provide a new path for producing advanced structure materials in which the deformation twinning works as one of the dominant plasticity mechanisms.

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