Cross‐Scale and Dynamic: Research Progress and Challenges in Precision Regulation of Electrocatalysis at the Atomic and Molecular Scales

Electrocatalysis plays a pivotal role in renewable energy conversion and environmental governance, enabling key processes such as water splitting, CO 2 reduction, and nitrogen fixation. Despite significant advancements, precise regulation of catalytic performance at the atomic and molecular levels remains a challenge. This review presents a cross‐scale, dynamic analytical framework that integrates active site engineering with interfacial microenvironment regulation, spanning inorganic solid catalysts and molecular catalysts. We summarize recent progress in structural and electronic modulation of active sites, interface microenvironment engineering, catalyst stability enhancement, molecular dispersion control, and complex reaction pathway elucidation. We highlight innovative strategies from inorganic catalysts—including single‐atom catalysts with tailored coordination environments, multi‐metal synergistic sites, defect engineering, and dynamic reconstruction—to molecular catalysts with precisely controlled dispersion states, electronic structures, and conformational dynamics. The review also discusses the roles of advanced in situ characterization and machine learning in resolving dynamic reaction mechanisms and accelerating catalyst design. Finally, we identify key challenges such as precise active site regulation, real‐time monitoring of dynamic interfacial processes, and long‐term stability, and outline future directions, including atomically precise catalyst design and dynamic interface regulation. These insights lay the foundation for developing next‐generation electrocatalysts with high activity, selectivity, and durability for sustainable energy applications.