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Joint enhancement on strength and toughness provides a cutting-edge research frontier for metals and alloys. Conventional strengthening methods typically lead to suppressed ductility and fracture toughness. In this study, large-scale atomic simulation on the fracture process is performed featuring nanocrystals embedded with nano-scaled twin boundaries (TBs). Four toughening mechanisms by nano-scaled TBs are identified:(i) crack blunting through dislocation accommodation along the nano-scaled TBs;(ii) crack deflection in a manner of intragranular propagation;(iii) daughter crack formation along the nano-scaled TBs that further enhances the toughness and (iv) curved TB planes owing to an excessive pileup of geometrically necessary dislocations. These toughening mechanisms jointly dictate the mechanical behavior of nano-structured materials, and provide insights into the application of nano-scaled TBs …