Polycyclic aromatic hydrocarbons (PAHs) are of major scientific concern owing to their widespread presence in environmental compartments and their potential toxicological effects on humans and biota. In this study, the adsorption capacity of natural (montmorillonite (Mt)), synthetic (Na-Mica-4), and modified (with octadecylamine and octadecyltrimethylamine (ODA-Mt, ODA-Mica-4, and ODTMA-Mt and ODTMA-Mica-4)) clays were assessed and compared for the removal of 16 PAHs. Materials were synthesized and characterized by X-Ray diffraction, Zeta potential, and Fourier-transform infrared spectroscopy. The results showed its correct preparation and the incorporation of PAHs in the structure of the clays after the adsorption tests. The proposed materials were effective PAH adsorbents, with adsorption percentages close to 100%, in particular those using Mt. Mt and Na-Mica-4 presented a better adsorption capacity than their organofunctionalized derivatives, indicating that the adsorption of PAHs may occur both in the surface part and in the interlayer. The proposed adsorbents take the advantage of being a low cost and highly effective. They can be an interesting alternative for wastewater treatment and soil remediation to prevent PAH contamination.