High-entropy intermetallic (HEI) nanocrystals have recently emerged as a promising class of multicomponent catalysts that combine the compositional complexity of high-entropy alloys with the structural precision of ordered intermetallics. This unique combination offers new opportunities to regulate atomic arrangement, surface structure, and catalytic behavior beyond what is achievable in conventional alloys or disordered high-entropy systems. In this Review, we discuss HEI nanocrystals from the perspectives of formation principles, synthetic strategies, and catalytic applications. We first outline the thermodynamic and kinetic factors that govern ordering in multicomponent nanoscale systems, and then summarize the emerging synthetic approaches for controlling phase selection, atomic ordering, and surface structure. We next examine representative electrocatalytic applications and discuss how ordering, multielement interactions, and structural evolution collectively influence activity and stability. Finally, we highlight four critical directions for future research, including growth mechanisms, facet control, atomic-scale structural identification and interatomic interactions, and electrocatalytic mechanisms. We anticipate that deeper insights into ordering, surface structure, and catalytic mechanisms will further expand the potential of HEI nanocrystals for a wide range of catalytic applications.




