RECENTLY, remarkable advances in amorphous alloys have been made because of the development of amorphous alloys having substantially high glass forming ability by conventional casting methods. [1][2][3][4] Among them, Zr-base amorphous alloys show superb glass forming ability [5] (critical cooling rate: about 1°C/s, maximum sample diameter: over 30 mm), excellent hardness, stiffness, strength, and corrosion resistance, [4,6] and thus have been applied to components of sporting goods and electrical products. However, they have poor ductility and toughness because brittle fracture readily occurs due to the formation of localized shear bands under tensile or compressive stress, [7] and have difficulties of fabrication of large structures or components, thereby limiting wide applications to advanced structural materials. Thus, if the fabrication of amorphous alloy/metal surface composites, in which the surface region consists of an amorphous alloy and the interior substrate consists of a ductile metal having sufficient ductility and fracture toughness, can be newly developed, the aforementioned problems of amorphous alloys can be solved while fully taking advantage of amorphous alloys. As a promising method to fabricate these amorphous alloy/metal surface composites, direct irradiation of highenergy electron beam is suggested.Upon irradiation on the metal substrate surface with highenergy electron beam, high kinetic energy of electrons, being struck into material lattices and forming phonons, is transformed to high thermal energy, which can easily melt alloys or ceramics with high melting points. When high-energy electron beam is irradiated on a metal substrate, where amorphous powders are evenly deposited, the substrate surface and amorphous powders are completely melted and solidified to form an amorphous alloy layer, thereby fabricating amorphous alloy/metal surface composites. This high-energy electron-beam irradiation has several advantages: (1) strong interfacial bonding between surface composite layer and substrate, (2) prevention of surface oxidation and intrusion of inclusions because of short irradiation time, (3) prevention of pores or cracks because of homogeneous heating and cooling, and (4) possible continuous processing of large-scale structures or parts because of working in air. [8] Compared with the laser beam method, this method has twice higher thermal efficiency, and produces a thicker surface composite layer of several millimeters in thickness.In this study, an amorphous alloy/copper surface composite was fabricated by depositing Zr-base amorphous powders on a copper substrate and irradiating them with a high-energy electron beam. In order to thicken a surface composite layer and to obtain a homogeneous microstructure, a two-layered surface composite was fabricated by repeating the electronbeam irradiation process, and its microstructure and hardness were analyzed in comparison with those of the one-layered surface composite fabricated by the one-time electron-beam irradiation.The Zr-base amorph...