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Both inorganic- and organic-pillared montmorillonites (PMts) were used to adsorb phenol to study suitable conditions for adsorption and adsorption isotherms. The adsorbing capacity of modified clays depends not only surface area, but mainly on micropore structure and surface components. After incandescing at 500°C, the pillar structure and the basal interlayer spacing (1.83 nm) remained stable. Using modified PMt with surfactant can improve adsorbing capacity greatly. The PMt can be recycled, and it is a potential substance for adsorption of environmental pollutants.