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DOI: 10.1002/adma. 201603880 catalysts for HER.[8–10] However, being best known for their superior mechanical properties, amorphous alloys or metallic glasses (MGs) have attracted intensive interests as structural materials rather than for functional applications.[11] Recently, through thermoplastic forming, Schroers and co-workers demonstrated the effectiveness of nanostructured MGs for electrochemical reactions.[8, 12, 13] Zhao et al.[14] and Yang et al.[15] also investigated the catalytic properties of MG nanoparticles and thin film for methanol electrooxidation and oxygen reduction reactions, respectively. Nevertheless, the application of MGs for HER is still blank. In this study, we report a multicomponent Pd40Ni10Cu30P20 MG catalyst, which not only exhibits excellent electrocatalytic activity but also possesses unique selfstabilizing catalytic performance over a long-cycling life. Such superior features of the amorphous catalyst originate from the self-optimized active sites, arising from the intrinsic chemical heterogeneity and the selective dealloying of elements on the multicompositional disordered surface, which uncover a new mechanism for improving the durability of catalysts. The Pd40Ni10Cu30P20 alloy, one of the best known metallicglass-formers,[16] was fabricated by arc melting and single-roll melt-spinning techniques in ribbons (Supporting Information). X-ray diffraction, differential scanning calorimetry, and high-resolution transmission electron microscopy analyses verify the amorphous structure of the ribbons (Figure S1, Supporting Information). A standard three-electrode configuration was used to evaluate the electrocatalytic …