Achieving homogeneous plastic deformation in metallic glasses is a long-standing goal yet to be solved in materials science.Here we investigate the effect of ion irradiation on the plastic deformation behavior of ZrCu/ZrCuNiAlSi amorphous/amorphous nanolaminates (A/ANLs) via nanoindentation testing.The experimental results indicate a dramatic change in deformation mode from multiple shear banding events to homogeneous compressive deformation before and after ion irradiation on the A/ANLs in the areas underneath the indenter.Ion irradiation-induced changes of both fraction and distribution of free volume inside each constituent layer and interfacial state in the A/ANLs may be responsible for the unusual homogeneous deformation behavior.Our results suggest that the mechanical property of A/ANLs could be modified by tuning both the inner and interracial structure via ion irradiation.