AbstractTransition‐metal‐based layered double hydroxides (TM‐LDHs) nanosheets are promising electrocatalysts in the renewable electrochemical energy conversion system, which are regarded as alternatives to noble metal‐based materials. In this review, recent advances on effective and facile strategies to rationally design TM‐LDHs nanosheets as electrocatalysts, such as increasing the number of active sties, improving the utilization of active sites (atomic‐scale catalysts), modulating the electron configurations, and controlling the lattice facets, are summarized and compared. Then, the utilization of these fabricated TM‐LDHs nanosheets for oxygen evolution reaction, hydrogen evolution reaction, urea oxidation reaction, nitrogen reduction reaction, small molecule oxidations, and biomass derivatives upgrading is articulated through systematically discussing the corresponding fundamental design principles and reaction mechanism. Finally, the existing challenges in increasing the density of catalytically active sites and future prospects of TM‐LDHs nanosheets‐based electrocatalysts in each application are also commented.