Water splitting driven by renewable energy sources is considered a sustainable way of hydrogen production, an ideal fuel to overcome the energy issue and its environmental challenges. The rational design of electrocatalysts serves as a critical point to achieve efficient water splitting. Layered double hydroxides (LDHs) with two-dimensionally (2D) layered structures hold great potential in electrocatalysis owing to their ease of preparation, structural flexibility, and tenability. However, their application in catalysis is limited due to their low activity attributed to structural stacking with irrational electronic structures, and their sluggish mass transfers. To overcome this challenge, attempts have been made toward adjusting the morphological and electronic structure using appropriate design strategies. This review highlights the current progress made on design strategies of transition metal-based LDHs (TM-LDHs) and their application as novel catalysts for oxygen evolution reactions (OERs) in alkaline conditions. We describe various strategies employed to regulate the electronic structure and composition of TM-LDHs and we discuss their influence on OER performance. Finally, significant challenges and potential research directions are put forward to promote the possible future development of these novel TM-LDHs catalysts.