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.