Algerian halloysite intercalated with dimethyl sulfoxide (DMSO) was prepared. The starting (H) and resulting (H-DMSO) materials were characterized by X-ray powder diffraction, Fourier transformed infrared spectroscopy, thermal analysis, transmission electron microscopy, pore-size distribution analysis, and employed as crystal violet (CV+) adsorbents from aqueous solutions. Intercalation reaches a rate of 95% and increases the basal spacing to 11.2 angstrom. (CH3)(2)SO interacts with the inner surface hydroxyls of halloysite through new hydrogen bonds with the S=O groups. The release of DMSO occurs in two phases: a partial elimination at 195 degrees C and a second part due to the DMSO combustion at 277 degrees C. The TEM image of H-DMSO reveals halloysite nanotubes (HNTs) polydisperse in length and diameter. A heterogeneous distribution in the nanotube size was highlighted with pore diameters of 10-11, 20.6, 28.6, and 37.0nm, in correlation with transmission electron microscopy. The Redlich-Peterson equation describes efficiently the CV+ adsorption onto the modified sample. H-DMSO adsorbs 93.6 against 50.9mgg(-1) for the starting material. This improving of the adsorption capacity of DMSO-intercalated HNTs, was explained via the behavior of the intercalated DMSO molecules. Intercalation constitutes a key procedure for developing new nanocomposites, attractive in technological applications, such as effective adsorbents.