A hexagonal mesoporous silica (HMS) and its postfunctionalized counterparts with propyl (P-HMS) and aminopropyl (AMP-HMS) were prepared and characterized by elemental analysis, N2 adsorption, powder x-ray diffraction, Fourier-transform infrared, and surface charge measurements. Batch experiments were further performed to systematically investigate adsorption properties of these materials toward two nonpolar aromatic compounds (pyrene and pentachlorobenzene) and three phenolic compounds (2,4-dichlorophenol, pentachlorophenol, and 4-methyl-2,6-dinitrophenol) in aqueous solutions. The adsorption isotherms were well described by the Freundlich model and varied in adsorption linearity. For HMS and P-HMS, the adsorption of pyrene and pentachlorobenzene was much stronger than that of pentachlorophenol at pH slightly greater than 6. Alternatively, for AMP-HMS, pentachlorophenol and 4-methyl-2,6-dinitrophenol showed comparable or stronger adsorption affinity than the other target compounds did, suggesting that a major role is played by electrostatic interactions of the two phenols. Furthermore, adsorption decreased with increasing pH for all adsorbate-adsorbent combinations except that of pentachlorophenol and 4-methyl-2,6-dinitrophenol on AMP-HMS, which showed bell-shaped curves with the maximum adsorption at pH close to the pKa. The advantages of reversible adsorption and fast adsorption/desorption kinetics (<15 min), as compared to commercial microporous activated carbons, make AMP-HMS a promising candidate to remove selected phenolic compounds in water treatment.