Electrochemical water splitting is regarded as a most effective hydrogen production technique. In fact, quite a few exceptional electrocatalysts, processes, and even large‐scale demonstrations have been developed. In particular, some amorphous catalysts have become well‐known for their extraordinary performance on account of their disordered structure, numerous, uniformly distributed active sites with high unit activity and better stability that outshine their single‐crystalline counterparts. Herein, a review of recent research advances of amorphous catalysts used in electrocatalytic water splitting are provided, including both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Particularly, the scaled‐up application of amorphous catalysts with multifarious compositions and diverse heterostructures in electrolyzing water and the reason why amorphous catalysts exhibit excellent catalytic performance are emphasized on. In addition, the mechanism of water electrolysis and the evaluation criteria of catalytic properties are analyzed in detail. Finally, the broader development outlook of amorphous catalysts is discussed.

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High‐entropy materials (HEMs) have been in the spotlight as emerging catalysts for electrochemical water splitting. In particular, HEM catalysts feature multi‐element active sites and unsaturated coordination as well as entropy stabilization in comparison with their single‐element counterparts. Herein, a comprehensive overview of HEM catalysts used in electrochemical water splitting is provided, covering both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Particularly, the review begins with discussions of the concept and structure of HEMs. In addition, effective strategies for rationally designing HEMs on the basis of computational techniques and experimental aspects is described. Importantly, the importance of computationally aided methods, that is, density functional theory calculations, high‐throughput screening, and machine learning, to the discovery and design of HEMs, is described. Furthermore, the applications of HEMs in the field of water electrolysis are reviewed. Eventually, an outlook regarding the prospects and future opportunities for HEMs is provided.

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