Nanoscale Tailoring of Bulk High Entropy Alloys for Structural and Functional Applications

ABSTRACT High‐entropy alloys (HEAs) represent a transformative class of materials whose exceptional mechanical and functional properties arise from their compositional complexity and adaptable microstructures. Recent advances in nanoscale tailoring of bulk HEAs—via grain refinement, hierarchical architecture, precipitation, and interface engineering—have unlocked unprecedented opportunities to simultaneously enhance strength, ductility, thermal stability, and multifunctionality. Structurally, nanograined, precipitation‐strengthened, and heterogeneous HEAs exhibit remarkable strength–ductility synergy through interface‐mediated strengthening, back‐stress hardening, and strain partitioning. Functionally, nanoscale design confers superior electrocatalytic activity, magnetic, magnetocaloric responsiveness, radiation tolerance, and improved thermoelectric performance. Despite these advances, challenges remain in scalable synthesis, structural uniformity, and predictive understanding of nanoscale deformation and phase evolution. Integrating in situ and operando characterization, multiscale modeling, and machine learning–driven informatics is accelerating the discovery and optimization of HEA nanostructures. This review highlights emerging strategies for translating nanoscale design principles into cost‐effective, application‐specific architectures for aerospace, nuclear, and energy conversion systems, demonstrating how nanoscale tailoring transforms bulk HEAs into structurally resilient and functionally adaptive materials for extreme environments.