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Irradiated waste high-density polyethylene@Zn/ionic liquid novel composite well-fabricated via coacervation method was irradiated by gamma-irradiation and studied the effect of that radiation on the desulfurization process. The prepared composites were characterized by various analytical techniques as follows: X-ray diffraction (XRD), Fourier-Transform infrared (FT-IR), X-ray photoelectron spectrometer (XPS), scanning electron microscope (SEM), High Resolution Transmission Electron Microscopy (HRTEM), N 2 -adsorption-desorption isotherm, and thermal gravimetric analysis (TG/DTA). The adsorptive desulfurization process of benzothiophene (BT) and dibenzothiophene (DBT) which are harmful compounds in diesel model fuel was investigating using the irradiated and unirradiated composite. The results illustrated that the unirradiated and irradiated composites exhibit an adequate adsorption capacity reached (50-75 mg S/g) and (60-85 mg S/g) for BT and DBT, respectively. The adsorption process over the prepared adsorbents follows the pseudo-second-order kinetic models. The irradiated composite exhibited more adsorption capacity than the unirradiated one due to the radiation generated more surface area and created proton-bond donor sites in the composite surface, which increases the interaction between the surface and sulfur species. The adsorption capacity and adsorption percentage for irradiated and unirradiated composites towards (SCCs) were studied using response surface methodology based on the central composite design (CCD). The thermodynamic factors (∆H°, ∆G°, and ∆S°) reveal that these processes are endothermic adsorption processes. The irradiated PEt @Zn/IL was re-used without significant loss of adsorption activity. This novel irradiated PEt @Zn/IL is the first time used as an adsorbent with an advantage that includes its excellent adsorption capacity, which ensures the product will be efficient in a real process such as the petrochemical industry., (© 2021. The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.)