<p>This work presents a sustainable and eco-friendly method using covalent organic frameworks (COFs) under visible light to selectively photocatalyze the oxidation of aromatic alcohols into beneficial aromatic aldehyde compounds. Under mild conditions, this work investigated a composite of CuBi₂O₄ and CTFs (CTF-CuBi₂O₄) as a heterogeneous photocatalyst for the oxidation of benzyl alcohols to their respective benzaldehydes using TBHP as the oxidizing agent. Several microscopic and spectroscopic techniques, including FT-IR, PXRD, SEM, TEM, EDAX, BET, TGA, UV-DRS, Matt-Schottky, and PL, were used to investigate the physical and structural features of this photocatalyst. Moreover, mass spectroscopy, ¹H NMR, and¹³C NMR were the techniques applied to verify the corresponding benzaldehydes’ structures. The target products can be synthesized in moderate to high yields under appropriate reaction conditions. This technology offers advantages such as diminished reaction time and temperature (room temperature), utilization of visible light as a renewable and eco-friendly energy source, moderate reaction conditions, application of a recyclable catalyst, enhanced selectivity, and minimized undesirable byproducts. Additionally, the stability and recyclability of the catalyst were examined under ideal conditions, revealing that it can be reversibly reused for up to 6 cycles without substantial loss of activity.</p>