Dual‐Enhancement Strategy for <scp>OER</scp> via Ni–Co–Fe Tri‐Level Electron Regulation and La‐Assisted Structural Stabilization: <scp>L</scp> a <scp>F</scp> e Selective Coating on <scp>C</scp> o <scp>CH</scp> / <scp>NF</scp> Precatalyst

The oxygen evolution reaction suffers from sluggish kinetics and poor structural stability, necessitating the development of nonprecious metal electrocatalysts with efficient electronic regulation and intrinsic structural robustness. Herein, we construct a composite precatalyst of LaFe species modified cobalt carbonate hydroxide supported on nickel foam (LaFe–CoCH/NF) through a three‐step process involving electrodeposition, hydrothermal growth, and co‐deposition. This strategy enables the formation of a Ni–Co–Fe tri‐level electron regulation pathway coupled with a spatially selective LaFe coating layer, achieving dual enhancement in both electronic modulation and structural stabilization. The hierarchical electron pathway effectively activates Ni sites within the nickel foam substrate, promotes the generation of high‐valence Ni and Co species, and simultaneously suppresses the overoxidation of Fe. Meanwhile, the La‐induced local electric field and buffering effect alleviate the detachment of the active phase during electrochemical reconstruction. As a result, the optimized LaFe–CoCH/NF catalyst exhibits outstanding oxygen evolution reaction performance, with a low Tafel slope of 33.75 mV dec −1 and exceptional durability, maintaining over 1500 h of stable operation at 10 mA cm −2 , continuous operation for 1200 h at 50 and 100 mA cm −2 , and more than 200 h of durability even at an ultrahigh current density of 500 mA cm −2 . Mechanistic investigations reveal that the tri‐metallic electron regulation strategy significantly improves interfacial charge transfer efficiency and structural integrity, offering theoretical guidance and a viable design route for advanced multi‐metallic oxygen evolution reaction precatalysts.