Metallic glasses with a disordered atomic structure possess many appealing properties that are unachievable from crystalline counterparts. [19,20] Particularly, the metastable and defective nature of metallic glasses offers unique chemical activities, while the structural and chemical homogeneities give rise to outstanding corrosion resistance in acidic and alkaline electrolytes although metallic glasses are thermodynamically unstable. [21,22] Historically, the catalysis of metallic glasses has been extensively investigated for various chemical and electrochemical reactions since 1980s. [23][24][25][26][27] However, most catalytically active metallic glasses are noble metal-based alloys, such as PdSi and PdGe alloys, and the catalytic applications were restricted by insufficient catalytic activities, poor catalytic efficiency, high materials costs, and narrow composition ranges for glass formation and chemical modification. On the other hand, economic transition metalbased metallic glasses, such as NiFeP, have also been widely studied but with focus on magnetic and mechanical properties. [28] In the last two decades significant progress in understanding structure and glass forming ability of metallic glasses has been achieved with the finding of the multicomponent alloying effect. [29,30] A large number of noble-metal-free metallic glasses with a widely tunable chemical composition, which can satisfy various chemical demands, have been developed. The combination of metastable characteristics, widely tunable compositions, and high corrosion resistance makes metallic glasses very promising catalytic materials.Inspired by the recent findings of catalytically active metal phosphides, [31][32][33][34][35] in this study we report a new water splitting catalyst, Ni 40 Fe 40 P 20 metallic glass, toward high efficiency HER and OER in acidic and basic electrolytes (Figure 1a). The novel glassy catalyst exhibits unusual bulk catalysis with low onset potentials, small Tafel slopes, and excellent stability, which are comparable to or even better than the state-of-theart Pt and IrO 2 catalysts that are currently used in commercial electrolyzers.The metallic glass Ni 40 Fe 40 P 20 (at%) ribbons were prepared by a melt spinning method under a high-purity argon atmosphere (Figure 1b). The alloying composition is optimized based on two criteria: glass forming ability and catalytic activity. The as-prepared ribbons are ≈1-3 mm wide, 20-30 μm thick, and tens of centimeters long (Figure 1b; Figure S1, Supporting Information). The flexible ribbons can be cut and bent to any length and shape for direct device applications. The Many transition metals and alloys are expected to have high catalytic activities because of incompletely filled d orbitals for readily giving and taking electrons. However, the poor corrosion resistance, originating from high chemical activity, limits their applications as electrocatalysts for reactions in acidic and alkaline electrolytes. In this study, it is found that homogeneous amorphous structure can ef...