Organo-montmorillonites (OMts) modified by cationic surfactant (hexadecyltrimethylammonium bromide, C16) and zwitterionic surfactant (hexadecyldimethyl (3-sulphonatopropyl) ammonium, Z16) were used to remove phenol and Cu(II) from aqueous solution. The OMts were characterized by X-ray diffraction (XRD), thermogravimetric analysis (TG), Fourier-transform infrared spectroscopy (FTIR), X-ray fluorescence (XRF), and C, H, and N elemental analyses. Besides the independent adsorption of single contaminants, simultaneous and sequential adsorption of phenol and Cu(II) onto OMts were also investigated. The organic carbon contents of the two OMts were similar but the basal spacing of Z16 modified montmorillonite (Z16-Mt) was larger than that of C16 modified montmorillonite (C16-Mt) indicating a higher packing density of surfactant and hydrophobicity in C16-Mt with a slight higher adsorption capacity toward phenol. On the other hand, C16-Mt showed much lower capacity in adsorbing Cu(II) as compared with raw montmorillonite. On the contrary, the adsorption capacity of Z16-Mt toward Cu(II) was comparable with that of raw montmorillonite. The equilibrium data of phenol and Cu(II) were fitted satisfactorily with Linear and Langmuir models, respectively. In the sequential adsorption system, the adsorption of one contaminant was not affected by the other pre-adsorbed one; desorption of pre-adsorbed contaminant was also investigated. For both two contaminants, one did not affect the adsorption of the other one onto Z16-Mt and C16-Mt in the simultaneous system. Z16-Mt could rapidly and efficiently remove both phenol and Cu(II) simultaneously. The adsorption kinetics followed the Pseudo-second order model. The results of this work might provide novel information for developing new effective adsorbents toward organic contaminants and heavy metals. (C) 2015 Elsevier B.V. All rights reserved.