2D metal (hydr)oxide nanosheets have captured increasing interest in electrocatalytic applications aroused by their high specific surface areas, enriched chemically active sites, tunable physiochemical properties, etc. In particular, the electrocatalytic reactivities of materials greatly rely on their surface electronic structures. Generally speaking, the electronic structures of catalysts can be well adjusted via controlling their morphologies, defects, and heterostructures. In this Review, the latest advances in 2D metal (hydr)oxide nanosheets are first reviewed, including the applications in electrocatalysis for the hydrogen evolution reaction, oxygen reduction reaction, and oxygen evolution reaction. Then, the electronic structure–property relationships of 2D metal (hydr)oxide nanosheets are discussed to draw a picture of enhancing the electrocatalysis performances through a series of electronic structure tuning strategies. Finally, perspectives on the current challenges and the trends for the future design of 2D metal (hydr)oxide electrocatalysts with prominent catalytic activity are outlined. It is expected that this Review can shed some light on the design of next generation electrocatalysts.