Abstract: A new magnetic nanocatalyzed synthetic method for the synthesis of aldimines was demonstrated. The reaction was carried out in a Schlenk tube under reflux conditions using various solvents and different nanomaterials as catalysts. In these reactions, an excellent yield of aromatic aldimines was afforded in the presence of silica-coated magnetic nanomaterials. The prepared catalyst was also characterized by Fourier transform infrared (FT-IR) spectroscopy, scanning electron microscopy (SEM), nitrogen adsorption and desorption studies (BET), energy dispersive X-ray (EDX) and small-angle X-ray scattering (SAXS). It was shown that the magnetic nanocatalysts can be easily separated from the reaction mixture by an external magnet and reused.