The extensive consumption of freshwater resources and the continuous discharge of pharmaceutical residues pose serious risks to aquatic ecosystems and public health. In this study, pristine ZnO, TiO₂, Zn@TiO₂, and Ti@ZnO nanocomposites were synthesized via a precipitation-assisted solid–liquid interference method and systematically evaluated for the photocatalytic degradation of the antibiotic levofloxacin under UV and visible light irradiation. The structural, optical, and surface properties of the synthesized materials were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), UV–visible diffuse reflectance spectroscopy (UV–DRS), and X-ray photoelectron spectroscopy (XPS). XRD analysis confirmed the crystalline nature of all samples, while SEM images revealed spherical and agglomerated morphologies. Photocatalytic experiments were conducted using a 50-ppm levofloxacin solution with a catalyst dosage of 1 g L⁻¹. Pristine ZnO exhibited limited visible-light activity (33.81%) but high UV-driven degradation (92.98%), whereas TiO₂ showed comparable degradation efficiencies under UV (78.6%) and visible light (78.9%). Notably, Zn@TiO₂ nanocomposites demonstrated superior photocatalytic performance, achieving over 90% and near 70% degradation under both UV and visible light, respectively, while Ti@ZnO composites exhibited less than 60% degradation. The enhanced activity of Zn@TiO₂ is attributed to improved interfacial charge transfer, suppressed electron–hole recombination, and extended light absorption. These findings highlight Zn@TiO₂ nanocomposites as promising photocatalysts for efficient treatment of pharmaceutical wastewater under dual-light irradiation.