Gibbs free energy (ΔG) of water splitting reaction is 237.2 kJ mol −1 , corresponding to a theoretical voltage of 1.23 V. [3] However, the existence of electrochemical/concentration polarization and solution resistance can increase the actual voltage of water electrolysis to much beyond 1.23 V. Particularly, the OER involves a complicated four-electron transfer process, which results in a sluggish kinetics thus has long been the bottleneck. [4] Therefore, it is necessary to explore efficient and robust electrocatalysts to reduce the overpotential of water electrolysis and the extra electric energy consumption. Although noble electrocatalysts, such as Pt, RuO 2 and IrO 2 , are recognized as the most efficient electrocatalysts for water electrolysis, their high scarcity and instability severely impede large-scale applications. [5] Recently, considerable effort has been focused on nonnoble transition-metal materials as viable alternatives for water splitting. Understanding the intrinsic catalytic mechanism and real active sites of these catalysts will benefit the rational design and application of high-efficiency catalysts.With the development of in situ characterization technologies, more reports have revealed that the original electrocatalyst (so-called "pre-catalyst") surface sites would undergo dynamic reconstruction and transform into real reactive species. [6] This in situ reconstruction process could tune the electrocatalytic behaviors such as adsorption, activation, and desorption, thus improving the catalytic performance. [7] On this basis, many researchers utilized the pre-reconstruction of electrocatalysts to obtain a large number of active species for the catalytic reactions. [8] It has been found that the intrinsic properties of the pre-catalysts, such as composition, atomic arrangement, porosity, and crystallinity, would affect the reconstruction rate, reconstruction degree, and catalytic activity of the reconstructed species. [9] Moreover, the reaction conditions also affect the reconstruction process, such as electrochemical operation, applied potential, electrolyte concentration, and pH. [6a] Therefore, tuning the reconstruction process to generate abundant active sites with high intrinsic activity is an effective strategy to boost the catalytic performance of electrocatalysts.Although some influential review articles on the reconstruction of catalysts during water electrolysis have emerged, [10] most of them focus on the discovery and characterization of the reconstruction phenomenon, less on the regulation of the reconstruction process. In addition, reconstructed catalysts for Water electrolysis is regarded as an efficient and green method to produce hydrogen gas, a clean energy carrier that holds the key to solving global energy problems. So far, the efficiency and large-scale application of water electrolysis are restricted by the electrocatalytic activity of applied catalysts. Recently, the reconstruction phenomenon of electrocatalysts during a catalytic reaction has been discovered, which ...