The Ni(II) complex of N-2,N-6-bis(3-(triethoxysilyl)propyl)pyridine-2,6-dicarboxamide (PDCA) has been prepared in situ and immobilized on MCM-41 to prepare a heterogeneous catalyst. Techniques such as FT-IR, low angle powder XRD, TGA, SEM, TEM, MP-AES, and N-2 sorption studies were used for characterization of the isolated heterogeneous catalyst, MCM-41@PDCA-Ni. MCM-41@PDCA-Ni was used for the synthesis of benzimidazoles and quinazolinones in coupling reaction of substituted benzaldehyde with o-phenylenediamine and anthranilamide, respectively. The new catalyst showed tolerance towards both electron-withdrawing and electron-donating functional groups present in benzaldehyde. The high yield, easy recovery, and reusability for five times without significant loss in catalytic efficiency are the main advantages of MCM-41@PDCA-Ni.