Sorption equilibrium of phenol and aniline onto the granular activated carbon and hyperreticulated un-functionalized polymeric resin (MN200) was investigated in single and binary component aqueous systems. Higher loading was obtained for aniline than phenol onto both sorbents, which is probably due to hydrophobic difference between both solutes and the greater electronic density of the aromatic ring of the aniline. Granular activated carbon reported larger uptake than resin MN200 for both solutes, which may be attributed to the better physical properties of the granular activated carbon, for instance, larger surface area. The experimental sorption could be properly described by the Langmuir and Freundlich isotherms. Five models for predicting the binary equilibrium sorption isotherm were compared in order to determine the best fit model to correlate binary experimental data: the extended Langmuir isotherm with and without a constant interaction factor, a simplified model based on the single equilibrium factors, the empirical extended Freundlich isotherm and the modified extended Langmuir equation, which considers the synergistic interactions between sorbate-sorbate and not only the competition between them defined by the extended Langmuir model. The modified extended Langmuir model provides the best agreement between predicted and experimental data indicating that the synergistic interactions between solutes play an important role in the binary phenol/ aniline sorption system.