The FT-IR and XRD: spectra of HDTMA-bentonite and BDMHDA-bentonite loaded with phenol were registered. As follows from the spectra and the equillibrium data phenol sorption on the clay modified by hexadecyltrimethylammonium cation (HDTMA+) or benzyldimethylhexadecylammonium cation (BDMHDA+) is satisfactory. The distribution constants of phenol Kd(phen) and phenolate anion Kd(phen)− are higher in the case of BDMHDA-bentonite than HDTMA-bentonite. This fact can be explained from the viewpoint of different arrangements of surfactant cations in the interlamellar space of bentonite, i.e. vertical and parallel arrangements in BDMHDA- and HDTMA-bentonite, respectively.