Metallic glasses (MGs) are known to have high strength, but poor ductility. Prior studies have shown that plasticity in MG can be enhanced by significantly reducing their dimension to nanoscale. Here we show that, via the introduction of certain types of crystalline/amorphous interfaces, plasticity of MG can be prominently enhanced as manifested by the formation of ductile “dimples” in a 2 μm thick amorphous CuNb film. By tailoring the volume fraction and architecture of crystalline/amorphous multilayers, tensile fracture surface of MG can evolve from brittle featureless morphology to containing ductile dimples. In situ micropillar compression studies performed inside a scanning electron microscope show that shear instability in amorphous layers can be inhibited by interfaces. The mechanisms for improving plasticity and fracture resistance of MG via interface and size effect are discussed.