High-entropy alloys (HEAs) contain five or more main elements, and each element ranges in content from 5% to 35%. Due to the abundant selectivity of elements, excellent structural stability, and adjustable active centers, HEAs have been widely used in electrocatalysis. Designing HEA catalysts at the atomic scale can deeply describe their structural complexity and accurately reflect the relationship between HEA structure and catalytic performance. In this Review, the atomic design of HEA-based electrocatalysts is introduced and it is evaluated in terms of activity, stability, selectivity, and efficiency. Ingenuity at the atomic level can customize the atomic composition and geometric structure of HEAs, thereby enhancing the intrinsic activity of the catalytic site, creating new active sites, and improving operational stability. The Review provides insights into excellent electrocatalytic properties and guidance for the design and synthesis of advanced HEA electrocatalysts from the viewpoint of atomic fabrication.