Background: The widespread presence of organic dyes in the various industries’ effluent such as paper, textile, and clothing has led to significant environmental pollution. Titanium oxide (TiO2 ) nanoparticles immobilized on zeolite (ZSM-5) were investigated under UV light for activation of peroxymonosulfate (PMS) for photocatalytic degradation of Orange II (OII) dye in aqueous solutions. Methods: In this study, the photocatalyst used was prepared by immobilizing different amounts of TiO2 nanoparticles on ZSM-5. Characterization analyses including X-ray diffractometer (XRD), Fourier transform infrared (FTIR), BET, scanning electron microscope (SEM), and energy dispersive X-ray spectroscopy (EDS) were performed on the synthesized samples. Then, the effect of various parameters, such as TiO2 nanoparticles loading onto the ZSM-5, pH, contact time, dye concentration, and TiO2 / ZSM-5 dosage, is investigated for the removal of OII as a model molecule under the UV irradiation with 15 W power. Results: The highest removal percentage of OII dye (97.44%) was obtained in the optimal operating conditions of pH=3, the initial dye concentration=5 ppm, amount of TiO2 /ZSM-5=10 mg/L, amount of PMS=50 mg/L, and reaction time=120 minutes. The Langmuir–Hinshelwood kinetics model fitted with the experimental data. Conclusion: The obtained results of this research showed that PMS can be used as a suitable oxidant activated with ZSM-5/TiO2 nanocomposite in OII degradation in different water environments, by optimizing the effective operating factors.