Metallic glasses (MGs), with high density of low coordination sites and high Gibbs free energy state, are novel promising and competitive candidates in the family of electrochemical catalysts. However, it remains a grand challenge to modify the properties of MGs by control of the disordered atomic structure. Recently, nanostructured metallic glasses (NGs), consisting of amorphous nanometer‐sized grains connected by amorphous interfaces, have been reported to exhibit tunable properties compared to the MGs with identical chemical composition. Here, it is demonstrated that electrodeposited Ni–P NG is characterized by an extremely high energy state due to its heterogeneous structure, which significantly promotes the catalytic performance. Moreover, the Ni–P NG with a heterogeneous structure is a perfect precursor for the fabrication of unique honey‐like nanoporous structure, which displays superior catalytic performance in the urea oxidation reaction (UOR). Specifically, modified Ni–P NG requires a potential of mere 1.36 V at 10 mA cm–2, with a Tafel slope of 13 mV dec–1, which is the best UOR performance in Ni‐based alloys. The present work demonstrates that the nanostructurization of MGs provides a universal and effective pathway to upgrade the energy state of MGs for the design of high‐performance catalysts in energy conversion.

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