Water splitting is an attractive method for sustainable hydrogen production. Owing to the sluggish kinetics of water reduction and oxidation, developing cost-effective catalysts is thus imperative and timely. Within this context, two-dimensional (2D) electrocatalysts represent a viable option, due to their unique properties, such as large surface area, ease of charge migration and mass transfer, and mechanical robustness during electrochemical reactions. In this review, we summarize the recent breakthroughs in the structure engineering of a range of 2D functional nanomaterials for boosting electrocatalytic water splitting, including transition metal oxides (TMOs), hydroxides (TMHs), sulfides (TMSs), phosphides (TMPs), metal-organic frameworks (MOFs), and others metal nitrides, carbides, and covalent organic frameworks (COF) and perovskite, etc.). In addition, we have also added a perspective that highlighting the promises and challenges in future research.