Nowadays, to alleviate the growing pressure of energy shortages and environmental pollution, electrochemical energy conversion is seen as a fossil‐free, secondary pollution‐free, and highly efficiency pathway. Electrocatalysts, as the “heart” of the electrochemical conversion process, play a key role in accelerating reaction rates and promoting efficiency. Transition‐metal‐based layered double hydroxides (TM LDHs), one of the famous electrocatalysts, show unique 2D supermolecular‐stratified structure, excellent electronic properties, and their raw materials are easily available. In this review, electrocatalysis‐related properties of TM LDHs and the state‐of‐the‐art synthesis methods of TM LDH‐based electrocatalysts are summarized. Modifications for promoting the development of TM LDH‐based electrocatalysts are included, such as carbon materials modification, defect engineering, and noble metal loading. Then, the application of TM LDH nanosheets in the field of electrocatalysis is reviewed in detail. Finally, recent challenges, ongoing improvements, and future expectations for TM LDH nanosheets are presented.

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