The natural vermiculite supplied from Weili miner of Xinjiang was submitted to an nitric acid treatment followed by calcinations, oxalic acid treatment, and sodium form by ion exchange, which results in the increase of the framework Si/Al ratio, the reduction of the layer charge density, and the conversion of the vermiculite into a form of sodium vermiculite. Then the Al pillared vermiculite was obtained by contact with the aluminum pillaring solution. Furthermore, phosphate sorption experiments were carried out for Al-pillared vermiculite under different conditions to investigate its sorption behaviors and mechanisms. The phosphate sorption maxima for the Al-pillared vermiculite are 98.0 % at pH3. Pseudo second order model can best describe the reaction rate, and the adsorption capacity calculated by the model is consistent with that actual measurement for Al-pillared vermiculite, which the correlation coefficient(R2)is 0.9961. The experimental data with phosphate concentrations from 0.5 to 5.0 mmol·L-1 follow Langmiur isotherm model for Al-pillared vermiculite. The increase of temperature from 10 ℃ to 60 ℃ increased the sorption of Pb(II), which indicates that the adsorption process is endothermic. The adsorption enthalpy is 5.583 kJ·mol-1, the entropy is 52.59 J·mol-1·K-1, and the free energy is –9.290 (10 ℃), -10.40 (30 ℃), -11.06 (45 ℃), -11.96 (60 ℃) kJ·mol-1 respectively.