Au Quantum Dots Anchored Y‐MOF Enabling Directional Interfacial Charge Transfer for Synergistic Redox Photocatalysis

ABSTRACT The synergistic photocatalytic production of hydrogen coupled with pollutant degradation offers a transformative pathway toward sustainable energy and environmental remediation. Here, a novel bifunctional photocatalyst was prepared by anchoring Au quantum dots (QDs) onto a pyrene‐derived yttrium‐based metal‐organic framework (Au/YT) using a one‐pot solvothermal approach. Notably, the optimized 2.0%Au/YT demonstrated an outstanding photocatalytic redox activity for H 2 production and toxic acetaldehyde (CH 3 CHO) removal simultaneously under visible light irradiation, surpassed 15.94‐ and 19.86‐times higher than that of original H 4 TBAPy counterpart. Comprehensive optical and electrochemical analyzes indicated that Au QDs significantly expand the light absorption range while also successfully speeding up the separation of photogenerated carriers. Meanwhile, the intrinsic multilayered structure of Y‐MOFs further synergizes with the anchored Au‐QD sites to establish metal–support interactions and augment charge transport dynamics, leading to a remarkable improvement in collaborative photocatalytic efficiency. Additionally, in situ XPS tests and DFT calculations substantiated a robust electronic interplay at the Au/YT interface, which effectually orchestrates directed interfacial charge migration and optimizes the adsorption/activation energy of reactant molecules. This work pioneers the development of dual‐functional rare earth‐based MOFs photocatalysts and furnishes fundamental insights into the rational design of synergistic redox photocatalysis systems tailored for clean solar energy production and environmental stewardship.