High-pressure homogenization was employed to incorporate formamide (FM) in palygorskite (Pal) for the fabrication of aminated hybrid materials. The interactions of FM molecules with Pal and the positions of FM molecules inside the structure of Pal after hybridization and heat treatments were investigated. It was found that high-pressure homogenization could improve the dispersion of Pal bundles and facilitate the additional incorporation of FM molecules into the tunnels or channels of Pal and that supported the formation of stable FM/Pal hybrid materials. Spectroscopic and thermal analysis results confirmed that FM molecules could attach to Pal via H-bonds. The tunnel of Pal remained perfect after calcination at 380 °C owing to the incorporated FM molecules. The adsorption capacity of the homogenized FM/Pal hybrid material towards Pb(II) (58.4 mg·g^− 1) was improved in comparison with the raw Pal (32.2 mg·g^− 1) after calcination at 380 °C. The enhanced interactions between the organic species and Pal structure via high-pressure homogenization provided an alternative strategy to design new stable hybrid materials.