Abstract High-entropy alloys (HEAs), with multi-principal-element composition, are gaining attention for their structural stability and mechanical properties. While extensive research has focused on using HEAs as electrocatalysts in the conversion of single-component reactions, such as hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), carbon dioxide reduction reaction (CO 2 RR), and so on. Their potential in the application of synergistic conversion of pollutants (for example, carbon dioxide (CO 2 ) and nitrogen oxides (NO x )) has been largely overlooked. This review overviews HEAs' fundamental concepts and characteristics, and delves into their advantages in transition metals and optimization strategies for the synergistic conversion process. It offers a novel approach for sustainable environmental remediation and resource utilization.