Abstract: Knoevenagel reaction catalysized by I2 loaded montmorillonite was developed using malonitrile and aromatic aldehyde as starting materials.Influences of catalysts,solvents and base on yields were screened using single factor methods and the temperature,reaction time,quivalency of starting materials were investigated using orthogonal tests.Yields up to 93.0% under the optimized conditoins.The products were characterized by 1H NMR,IR and M.P.Montmorillonite and molecular iodine has a synergistic catalytic effect which can be recycled three times.