Copper-based catalysts are widely employed in the catalytic conversion of aromatic compounds to phenolic derivatives. However, single-atom copper catalysts often exhibit limited reactivity and stability. In this study, we addressed these limitations by loading Cu onto NaY zeolite via ion exchange to synthesize a CuY catalyst, followed by Yb modification. By optimizing the Yb content, we significantly enhanced the anisole conversion rate and guaiacol yield. Catalyst characterization revealed that Yb species modulate the electronic structure of copper, favoring the formation of abundant Cu(+) species. This electronic modification promotes the catalytic generation of hydroxyl radicals (˙OH) from hydrogen peroxide, thereby accelerating the reaction kinetics. Furthermore, Yb incorporation into CuY induced the formation of oxygen vacancies, which improved hydroxyl radical adsorption and facilitated the generation of metal-oxo species. These synergistic effects collectively increased the reaction's overall conversion efficiency. Under optimized reaction conditions, the Yb/CuY catalyst achieved an anisole conversion of 56.2% and an ortho-selectivity of 74.6%, clearly outperforming previous reports.