A novel method for the modification of mesoporous silica, MCM-41, using an electrochemical approach has been developed, and the process was monitored by cyclic voltammetery and spectrometric methods. The method was applied to the modification of mesoporous silica with new functional groups which are not accessible by conventional methods. Malononitrile-functionalized MCM-41 mesoporous silica was characterized by low-angle X-ray diffraction, Fourier transform infrared spectroscopy, mass spectrometry, thermal analysis, elemental analysis, high resolution transmission electron microscopy, and surface area measurement (S (BET)). In addition, the application of malononitrile-functionalized MCM-41 as a sorbent for gold ions was demonstrated.