Vermiculite- and silica nanosheets-based adsorbents have received widespread attention due to the advantages of low cost, high efficiency, easy preparation and regeneration. In this study, vermiculite (Vt), silica nanosheets (SiNSs), organo-vermiculites (OVts) and organo-silica nanosheets (OSiNSs) modified by a series of asymmetric gemini surfactants [C22H45(CH3)2N+(CH2)sN+(CH3)2C6H13]Br2 (s is the spacer length, s = 2, 3, 6) were selected as adsorbents to study their adsorption behavior for removing cationic crystal violet (CV) and anionic methyl orange (MO) dyes. The structures and surface characters of adsorbents were revealed by various characterization techniques such as FT-IR, XRD, TG-DTG, SEM and EDS. From the results of adsorption experiments, SiNSs exhibited conspicuous adsorption towards cationic CV over Vt, OVts and OSiNSs, nevertheless, the adsorption capacity of 22-3-6-Vt for MO was superior to that of Vt, 22-2-6-Vt, 22-6-6-Vt, SiNSs and OSiNSs, which can be ascribed to the type of precursors, structures of adsorbents and dyes, charge characteristics of dye molecules and spacer length of the surfactants. qmax of CV on SiNSs reached 752.6 mg g−1 and that of MO onto 22-3-6-Vt attained 153.3 mg g−1. Furthermore, kinetics, isotherms and thermodynamics were executed for exploring retention mechanisms. The spent 22-3-6-Vt and SiNSs were regenerated by water and a mixture of 0.1 mol L−1 HCl solution and ethanol, respectively.