Palygorskite (PAL) was modified by a high-pressure homogenization assisted hydrothermal process. The effects of modification on the morphology, structure and physicochemical properties of PAL were systematically investigated by Field-emission scanning electron microscopy (FESEM), Transmission electron microscopy (TEM), Fourier transform infrared spectrometry (FTIR), Brunauer-Emmett-Teller (BET) analysis, X-ray diffraction (XRD) and Zeta potential analysis techniques, and the adsorption properties were systematically evaluated using Methylene blue (MB) as the model dye. The results revealed that the crystal bundles were disaggregated and the PAL nanorods became more even after treated via associated high-pressure homogenization and hydrothermal process, and the crystal bundles were dispersed as nanorods. The intrinsic crystal structure of PAL was remained after hydrothermal treatment, and the pore size calculated by the BET method was increased. The adsorption properties of PAL for MB were evidently improved (from 119 mg/g to 171 mg/g) after modification, and the dispersion of PAL before hydrothermal reaction is favorable to the adsorption. The desorption evaluation confirms that the modified PAL has stronger affinity with MB, which is benefit to fabricate a stable organic-inorganic hybrid pigment. (C) 2015 Elsevier B.V. All rights reserved.