Fe3O4 magnetic nanoparticles (MNPs) were functionalized by aminopropylsilane and reacted with aromatic aldehyde, and Fe3O4‐Si‐[CH2]3‐N=CH‐Aryl and Fe3O4‐Si‐(CH2)3‐NH‐CH2‐Aryl MNPs were prepared as novel magnetic nanocatalysts. Fourier transform infrared (FT‐IR), X‐ray diffraction (XRD), and scanning and transmission electron microscopy (SEM and TEM) were used to identify the MNPs. The catalytic activity of the MNPs was evaluated in the one‐pot synthesis of some novel poly‐substituted pyridine derivatives.