TiO2-pillared montmorillonite is successfully synthesized via sol-gel method, which is used to remove blue-green algae from water. The composite was characterized by X-ray diffraction and Scanning electron microscope. The analysis results shows that TiO2 has entered into the interlayer of montmorillonite and the d001 increases from 1.27639 nm to 1.64437 nm, and the surface charge of montmorillonite was recyanobacteriarkably raised from -41.5 mV (Fig. 1a) to +12.21 mV (Fig. 1b) mV at pH =6～8. The results of algae adsorption experiments displays the positive surface charge of modified montmorillonite was thus expected to induce the electrostatic neutralization between TiO2-pillared montmorillonite and Microcystis aeruginosa (CYANOBACTERIA) cells. When the cyanobacteria concentration is 12100 number/μL, chlorophyll content is 2.831883 mg/L, turbidity of the water is 44.2%, and TiO2-pillared montmorillonite is 0.5 g/L, the removing rate of chlorophyll and microcystis exceeds 90%, and the turbidity reduces from 44.2% to 19.1%.