The chemical surface of Santa Barbara Amorphous-15 (SBA-15) was functionalized with polyaniline (SBA-15/PA) and was prepared using aniline and ammonium persulfate as the modifying agent and oxidant. The samples were characterized by N2 physical adsorption at 77 K. SBA-15′s surface area was 654.5 m2 g−1, changing to 254.6 m2 g−1. The total acidity and basicity were determined using a modified Boehm’s method, and the point of zero charge pH (pHpzc) was determined. Immersion calorimetry in water, benzene, and NaOH, HCl, and phenol (100 mg L−1) solutions was performed, producing values ranging from −15.1 to −174.1 J g−1 related to the chemical surface, pHpzc, and acid and base group values. Finally, the phenol adsorption capacity was found to be higher for the modified polyaniline silica, at 138 mg g−1.