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Oxygen evolution reaction (OER) is a bottleneck to photoelectrochemical (PEC) water splitting; however, there remains an impressive challenge for intrinsic charge transport for the development of integrated photoanodes. Herein, covalent triazine frameworks as conjugated molecules are grafted on the surfaces of ferroelectric BaTiO3−x (CTF/BTO) nanorod array, and then oxyhydroxide oxygen evolution cocatalyst (OEC) is constructed as an integrated photoanode. The OEC/CTF/BTO array not only achieves a high photocurrent density of 0.83 mA cm−2 at 1.23 V versus reversible hydrogen electrode (vs RHE) and low onset potential of ≈0.23 VRHE, but also optimizes outstanding stability. To disclose the origin, the enhanced PEC activity can be contributed to the integration of CTF and OEC, enhancing light‐harvesting capability, boosting charge carrier mediation, and promoting water oxidation kinetics through electrochemical analysis and density functional theory calculations. This study not only provides an alternative to accelerate charge transfer, but also paves the rational design and fabrication of integrated photoanodes for boosting PEC water splitting performance. [ABSTRACT FROM AUTHOR]

Developing robust oxygen evolution reaction (OER) catalysts requires significant advances in material design and in‐depth understanding for water electrolysis. Herein, we report iridium clusters stabilized surface reconstructed oxyhydroxides on amorphous metal borides array, achieving an ultralow overpotential of 178 mV at 10 mA cm−2 for OER in alkaline medium. The coupling of iridium clusters induced the formation of high valence cobalt species and Ir–O–Co bridge between iridium and oxyhydroxides at the atomic scale, engineering lattice oxygen activation and non‐concerted proton‐electron transfer to trigger multiple active sites for intrinsic pH‐dependent OER activity. The lattice oxygen oxidation mechanism (LOM) was confirmed by in situ 18O isotope labeling mass spectrometry and chemical recognition of negative peroxo‐like species. Theoretical simulations reveal that the OER performance on this catalyst is intrinsically dominated by LOM pathway, facilitating the reaction kinetics. This work not only paves an avenue for the rational design of electrocatalysts, but also serves the fundamental insights into the lattice oxygen participation for promising OER application. [ABSTRACT FROM AUTHOR]