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The primary objective of this work was to investigate the simultaneous removal of refractory sulfur (dibenzothiophene, DBT) and nitrogen compounds (indole, IND) from model gasoline. This research aimed to develop an efficient adsorption process to mitigate the emission of sulfur oxide and nitrogen oxides, which pose direct threats to human health and the environment. Additionally, the study focused on addressing technical challenges encountered in the refinery process, particularly the poisoning of catalysts due to the presence of these compounds. To achieve the study's goals, granular activated carbon (GAC) was subjected to acid treatment for modification. Molybdenum species were then incorporated into the acid‐treated GAC using the wet impregnation technique. The composition and distribution of elements on the surface of the modified GAC (Mo‐AAC) were analyzed via X‐ray photoelectron spectroscopy (XPS). Various characterization techniques were employed to confirm the uniform dispersion of molybdenum species on the GAC surface. The specific surface area of the adsorbent was increased from 257 m2/g to 316 m2/g following the acid treatment and molybdenum modification. The study explored the impact of several key parameters on the removal of DBT and IND using central composite design (CCD). A regression model was derived using CCD through hybrid central composite design, and its adequacy was verified with the means of tests such as analysis of variance (ANOVA), a lack of fit test, and residuals distribution consideration. Experimental results match well with the results obtained by CCD model, justifying the accuracy of models. The results showed that all four parameters have a significant impact on removal of DBT and IND. Increasing temperature and the adsorbent dose positively affected the removal of both DBT and IND, indicating that higher temperatures and greater adsorbent dosages improved removal efficiency. On the other hand, the concentration of DBT and IND had a negative impact, signifying that higher initial contaminant concentrations hindered removal efficiency. The study determined the optimum initial contaminant concentrations for DBT and IND, temperature, and adsorbent dose to be 186 mg/L, 50 mg/L, 25.5°C, and 32 g/L, respectively. These conditions yielded the highest removal efficiency. The research demonstrated that Mo‐AAC has the capability to effectively reduce the sulfur and nitrogen content of model gasoline, making it a promising solution for addressing environmental and refinery challenges associated with these compounds. [ABSTRACT FROM AUTHOR]