A facile method was presented to disaggregate the crystal bundles of palygorskite (Pal) by combining the extrusion with high-pressure homogenization technique. The effects of extrusion times on the disaggregation degree of crystal bundles, the micro-structure and properties of Pal were investigated. Morphological characterization indicated that the crystal bundles were perfectly disaggregated without disrupting the rod-like single crystals after Pal extruded for three times and homogenized at 30 MPa. The specific surface area, micropore surface area, and micropore volumeof the corresponding Pal increased from175 m²/g, 31 m²/g, and 0.013 cm³/g (natural Pal) to 241 m²/g, 103 m²/g, and 0.048 cm³/g, respectively. Also, the viscosity of Pal dispersion increased from 152 mPa s (natural Pal) to 2976 mPa s.