A new and efficient procedure for the synthesis of 3,5‐disubstituted‐2,6‐dicyanoaniline derivatives by CoFe2O4@SiO2‐PA‐CC‐guanidine magnetic nanoparticles (MNPs) was reported. 3,5‐Disubstituted‐2,6‐dicyanoaniline derivatives were synthesized from malononitrile, aldehydes, and β‐nitrostyrene derivatives in good yields. MNPs used for the synthesis of aniline derivatives were easy to recover and reuse. The CoFe2O4@SiO2‐PA‐CC‐guanidine MNPs were characterized by Fourier‐transform infrared spectroscopy, scanning electron microscopy, energy‐dispersive X‐ray spectroscopy, X‐ray diffraction, thermogravimetric analysis, and vibration sample magnetometry techniques.