This study presents a simple, sustainable, eco-friendly approach for synthesizing copper oxide (CuO) nanoparticles using Citrus aurantium peel extract as a natural reducing and stabilizing agent. The synthesized CuO and CuO-OP were characterized using various techniques, including surface area measurement (S), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), diffuse reflectance spectroscopy (DRS), scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX), and high resolution transmission electron microscope (HRTEM). DRS analysis determines band gap energy (E) of 1.7 eV for CuO and 1.6 eV for CuO-OP. FTIR confirmed the presence of Cu-O bond groups. The XRD and HRTEM results revealed monoclinic and spherical nanostructures, with average particle sizes ranging from 53.25 to 68.02 nm, as determined via Scherer's equation. EDX analysis indicated incorporation of carbon (1.6%) and nitrogen (0.3%) from the peel extract. The synthesized CuO and CuO-OP NPs exhibited excellent photocatalytic efficiencies for methylene blue dye under UV irradiation, reaching 95.34 and 97.5%, respectively, under optimal conditions; the initial dye concentration was 100 mg/L, the pH was 10, the catalyst dosage was 1 g/L, and the contact time was 120 min. Isothermal studies showed that the adsorption of MB onto the nanoparticles followed the Freundlich isotherm model (R = 0.97 and 0.96). Kinetic studies indicated that the degradation followed pseudo-first-order kinetics, with rate constants (K) of 0.0255 min for CuO and 0.033 min for CuO-OP. The sorption capacities were calculated as 98.19 mg/g for CuO and 123.1 mg/g for CuO-OP. The energy values obtained from the Dubinin-Radushkevich isotherm were 707.11 and 912.87 KJ mol, suggesting that chemisorption was the dominant mechanism.