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The organophilization of clays to increase interfacial interactions is a typical practice when the objective is its encapsulation with a polymer. This work intend to synthesize and characterize an organo-palygorskite-Fe 3 O 4 , to change the hydrophilicity of the material and investigate its efficiency in the removal of two anionic dyes from aqueous solution with the aim to use this material to treat wastewater contaminated with dyes. The organophilization of modified palygorskite–Fe 3 O 4 was done with a cationic surfactant (cetyl trimethylammonium bromide, CTAB) and the material obtained was characterized by XRF, SEM, XRD, FTIR, Nano Zetasizer, density, BET surface area, TGA/DTA and contact angle measurements. XRF and FTIR confirmed the presence of carbon in the modified palygorskite–Fe 3 O 4 nanoparticles while XRD showed new crystalline phases from CTAB. Furthermore, a positive zeta potential value appeared and an inversion in the nanoparticles' hydrophobicity happened due to the increase of organic carbon content in the organo-palygorskite-Fe 3 O 4 . The adsorbed anionic dye on organo-palygorskite-Fe 3 O 4 may be completely recovered by the action of a magnet, showing an excellent adsorptive property and economical alternative adsorbents to treat dye wastewater. The negative values calculated for the free energies of adsorption indicate that the adsorption of methyl orange and indigo carmine on the active sites of organo-palygorskite-Fe 3 O 4 surface was spontaneous and that the indigo carmine had the best interaction with the magnetic organo clay. [ABSTRACT FROM AUTHOR]