The study published in Small delves into the use of high-entropy alloys (HEAs) in conjunction with semiconductor materials like TiO₂ to enhance photocatalytic hydrogen production. By synthesizing Pd-enriched HEA nanocrystals supported on TiO₂, researchers aimed to improve the performance of photocatalysts by exploring multielement compositions and their effects on interfacial properties and charge dynamics. The research focused on creating Pd@HEA core–shell nanocrystals with precise composition control and uniform particle size, which were then integrated into TiO₂ to form hybrid photocatalytic systems. Various analytical methods such as UPS, TAS, XPS, and DFT simulations were employed to understand the structure-function relationship, charge carrier dynamics, and active sites within the nanocrystals. Results showed that the HEA-coated samples exhibited higher hydrogen production efficiency, attributed to the formation of effective Schottky junctions with TiO₂, leading to improved charge separation. The study emphasized the role of multiple elements like Pd, Ir, Rh, Ru, and Pt in optimizing hydrogen adsorption energies and catalytic activity. Theoretical simulations highlighted the influence of multielement interactions on electronic structure and charge transfer pathways. Overall, the research underscores the promising prospects of utilizing high-entropy alloys and semiconductors for advancing photocatalytic hydrogen production.