Abstract A disordered crystal structure is an asymmetrical atomic lattice resulting from the missing atoms (vacancies) or the lattice misarrangement in a solid‐state material. It has been widely proven to improve the electrocatalytic hydrogen evolution reaction (HER) process. In the present work, due to the special physical properties (the low evaporation temperature of below 900 °C), Zn is utilized as a sacrificial component to create senary PtIrNiCoFeZn high‐entropy alloy (HEA) with highly disordered lattices. The structure of the lattice‐disordered PtIrNiCoFeZn HEA is characterized by the thermal diffusion scattering (TDS) in transmission electron microscope. Density functional theory calculations reveal that lattice disorder not only accelerates both the Volmer step and Tafel step during the HER process but also optimizes the intensity and distribution of projected density of states near the Fermi energy after the H 2 O and H adsorption. Anomalously high alkaline HER activity and stability are proven by experimental measurements. This work introduces a novel approach to preparing irregular lattices offering highly efficient HEA and a TDS characterization method to reveal the disordered lattice in materials. It provides a new route toward exploring and developing the catalytic activities of materials with asymmetrically disordered lattices.

Lattice‐Disordered High‐Entropy Alloy Engineered by Thermal Dezincification for Improved Catalytic Hydrogen Evolution Reaction