Gold (Au)-based nanomaterials, including nanoparticles (NPs) and nanoclusters (NCs), have shown great potential in many electrocatalytic reactions due to their excellent catalytic ability and selectivity. In recent years, Au-based nanostructured materials have been considered as one of the most promising non-platinum (Pt) electrocatalysts. The controlled synthesis of Au-based NPs and NCs and the delicate microstructure adjustment play a vital role in regulating their catalytic activity toward various reactions. This review focuses on the latest progress in the synthesis of efficient Au-based NP and NC electrocatalysts, highlighting the relationship between Au nanostructures and their catalytic activity. This review first discusses the parameters of Au-based nanomaterials that determine their electrocatalytic performance, including composition, particle size and architecture. Subsequently, the latest electrocatalytic applications of Au-based NPs and NCs in various reactions are provided. Finally, some challenges and opportunities are highlighted, which will guide the rational design of Au-based NPs and NCs as promising electrocatalysts.