Antibiotic contamination of water, particularly tetracycline (TC), poses significant environmental risks and requires sustainable treatment solutions. This study reports a green and cost-effective synthesis of a ZnO/chitosan nanocomposite (ZnO/CS) for photocatalytic TC removal. ZnO nanoparticles were synthesized using lime juice as a natural stabilizing agent and subsequently incorporated into a chitosan matrix. The physicochemical properties of the composite were characterized by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), UV–Vis diffuse reflectance spectroscopy (UV–Vis DRS), scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (SEM–EDX), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Brunauer–Emmett–Teller (BET) surface area analysis. The results confirmed the formation of hexagonal wurtzite ZnO and strong interfacial interactions between ZnO and the –NH2/–OH groups of chitosan. A red shift reduced the band gap from 3.18 to 3.03 eV, while the specific surface area increased from 10.7 to 21.7 m² g⁻¹. Under LED irradiation, the ZnO/CS nanocomposite achieved 94% TC removal within 120 min, following pseudo-first-order kinetics based on the Langmuir–Hinshelwood model. These findings demonstrate the potential of the green-synthesized ZnO/CS nanocomposite for antibiotic removal from aqueous environments.