The presence of sulfur compounds in fossil fuels has been an important concern in recent decades as an environmental risk due to the increase of greenhouse gases in the atmosphere and accentuation of acid rain. This study evaluates modified clays as low-cost and efficient adsorbents for the removal of dibenzothiophene (BT) and 4,6-dibenzothiophene (DBT). Adsorption was investigated in a batch system with synthetic fuels (gasoline and diesel) as a function of type of clay modification, adsorbent dosage, initial concentration of the pollutants, desorption, and isotherm modeling. Maximum adsorption was observed with clays modified with benzyltrimethylammonium ion (BM), achieving a maximum adsorption capacity (qmax) of BT of 11.3 mg/g in gasoline and 31.3 mg/g in diesel. The formation of Van der Waals interaction as well as aromatic forces as the main mechanism is proposed based on the results. A 40% desorption was accomplished in 0.1 N HCl. Adsorbents were characterized by scanning electron microscopy (SEM) and Fourier transform-infrared spectroscopy (FT-IR), indicating their optimum properties as adsorbents in fuels. This work highlights the potential use of reverse polarity clays in the elimination of sulfur compounds from model fuels as a low-cost and environmentally friendly purification technique.