M esoporous silica containing specific functional groups having a high specific surface areas and porosities that open ed a wide field of applications in removal of toxic metal ions from waste water and natural waters [1]. Thus they provide a suitable approach to the development of green chemistry principles. The importance of zirconium as a homogeneous catalyst has alread y been cited in the number of biologically and pharmaceutically significant organic transformations [2, 3]. Herein we have reported the importance of zirconium modified MCM 41 as a heterogeneous catalyst for the Knoevenagle condensation reaction of various aldehydes with malononitrile in water at 35 o C