Acid-activated clays are inexpensive materials that are used extensively in the removal of unsaturated compounds on an industrial scale. The performance of bentonitic clays in removing these compounds relies heavily on the types of raw clays and acids used in the activation process. In this work, we report on the removal of olefins from aromatic streams by bentonitic clays activated via two different routes. After preliminary tests of four different natural clays, the best clay was selected in terms of it having high swelling index, cation-exchange capacity, specific surface area and suspension stability values. Activation was achieved with hydrochloric acid (HCl) and sulfuric acid (H2SO4), and olefin removal was evaluated after holistic clay characterization by means of X-ray diffraction, X-ray fluorescence, Brunauer–Emmett–Teller (BET) specific surface area analysis, ζ-potential analysis, Fourier-transform infrared (FTIR) spectroscopy after treatment with pyridine, scanning electron microscopy and transmission electron microscopy. The increased basal spacing, replacement of H+ with interlayer cations and retained structural stability of the clay after acid treatment contributed to the improvement of olefin removal for HCl-activated clay. The HCl-activated clay was more efficient in terms of olefin removal than its H2SO4-activated counterpart, removing up to 90% of olefin components after 40 h. Based on pyridine-FTIR spectra and quantitative measurement of the acidic properties of the samples, HCl treatment increased the total number acid sites (Brønsted and Lewis) by approximately ninefold compared to the pristine natural clay and by approximately fourfold compared to the H2SO4-activated clay.