摘要:Metallic glasses are lucrative engineering materials owing to their superior mechanical properties such as high strength and great elastic strain. However, the Achilles' heel of metallic amorphous materials — low plasticity caused by instantaneous catastrophic shear banding, significantly undercut their structural applications. Here, the nanolayered crystalline Cu/amorphous Cu-Zr micropillars with equal layer thickness spanning from 20–100 nm are uniaxially compressed and it is found that the Cu/Cu-Zr micropillars exhibit superhigh homogeneous deformation (≥ 30% strain) rather than localized shear banding at room temperature. This extraordinary plasticity is aided by the deformation-induced devitrification via absorption/annihilation of abundant dislocations, triggering the cooperative shearing of shear transformation zones in glassy layers, which simultaneously renders the work-softening. The synthesis of such heterogeneous nanolayered structure not only hampers shear band generation but also provides a viable route to enhance the controllability of plastic deformation in metallic glassy composites via deformation-induced devitrification mechanism.