In this paper, palygorskite/alumina composite materials were prepared as the adsorbent by using sol-gel technique, and the adsorption properties and mechanisms of complex adsorbing phosphate were investigated, with a discussion on the adsorption kinetics and thermodynamic characteristics. The results demonstrate that the adsorption processes of phosphate on complex surface follow the pseudo-second-order equation most effectively and the rate constant increases with decreasing initial concentration and the rise of temperature. The adsorption isotherms fit Langmuir equation and D-R equation fairly well. The adsorption enthalpy is positive and the adsorption Gibbs free energy changes are in the range of-25～-21 kJ/mol. The adsorption process is endothermic and spontaneous, with the coexistence of physical adsorption and chemical adsorption.