Zr(IV)‐salen‐MCM‐41 was prepared by reaction of NH2‐MCM‐41 with salicylaldehyde to afford Schiff base ligands. Thereafter, ZrOCl2·8H2O was reacted with the Schiff base ligands for complex formation. The structural properties of the synthesized materials were investigated by a number of analytical techniques including X‐ray diffraction, N2 sorption‐desorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, inductively coupled plasma atomic emission spectroscpopy, and energy dispersive X‐ray spectroscopy. Catalytic studies of the mesoporous materials functionalized with Zr(IV)‐Schiff base complexes were investigated and extended to selective oxidation of sulfides to sulfoxides and the Knoevenagel condensation reactions of aldehydes with malononitriles and ethyl cyanoacetate. Additionally, catalyst recycling of the Zr‐salen‐MCM‐41 materials was also studied.