High‐entropy alloys (HEAs) have emerged as a groundbreaking class of materials poised to revolutionize solid‐state hydrogen storage technology. This comprehensive review delves into the intricate interplay between the unique compositional and structural attributes of HEAs and their remarkable hydrogen storage performance. By meticulously exploring the design strategies and synthesis techniques, encompassing experimental procedures, thermodynamic calculations, and machine learning approaches, this work illuminates the vast potential of HEAs in surmounting the challenges faced by conventional hydrogen storage materials. The review underscores the pivotal role of HEAs' diverse elemental landscape and phase dynamics in tailoring their hydrogen storage properties. It elucidates the complex mechanisms governing hydrogen absorption, diffusion, and desorption within these novel alloys, offering insights into enhancing their reversibility, cycling stability, and safety characteristics. Moreover, it highlights the transformative impact of advanced characterization techniques and computational modeling in unraveling the structure–property relationships and guiding the rational design of high‐performance HEAs for hydrogen storage applications. By bridging the gap between fundamental science and practical implementation, this review sets the stage for the development of next‐generation solid‐state hydrogen storage solutions. It identifies key research directions and strategies to accelerate the deployment of HEAs in hydrogen storage systems, including the optimization of synthesis routes, the integration of multiscale characterization, and the harnessing of data‐driven approaches. Ultimately, this comprehensive analysis serves as a roadmap for the scientific community, paving the way for the widespread adoption of HEAs as a disruptive technology in the pursuit of sustainable and efficient hydrogen storage for a clean energy future.
