Design Frontiers of High‐Entropy Materials for Advanced Electrocatalysis

Abstract High‐entropy materials (HEMs) have rapidly emerged as promising candidates for electrocatalysis owing to their highly tunable multi‐component systems and distinctive effects, including high‐entropy stabilization, lattice distortion, sluggish diffusion, and cocktail effects. To accelerate their advancement, rational design strategies and practical implementation guidelines are urgently required. This review first outlines advanced synthetic approaches from a thermodynamic perspective, offering pathways for constructing HEMs with tailored conformational relationships. It then presents a comprehensive overview of cutting‐edge design strategies, emphasizing component modulation, size and dimensionality control, morphology engineering, crystal facet regulation, phase engineering, and defect/strain engineering. Furthermore, the integration of machine learning and theoretical computation is discussed as a powerful tool to unravel complex structure–property relationships and to guide the efficient discovery of next‐generation HEMs. Finally, the applications of HEMs in small‐molecule conversion and their dynamic structural evolution phenomena are systematically summarized, highlighting key design principles underpinning their outstanding catalytic performance. Overall, this review provides a forward‐looking guideline for the rational design of HEM‐based electrocatalysts, with the aim of advancing efficient and sustainable energy conversion technologies.