Chitosan-coated Fe3O4 nanoparticles (Fe3O4@CS) were prepared simply through in situ co-precipitation of Fe2+ and Fe3+ ions via NH4OH in an aqueous solution of chitosan and their catalytic activity was investigated in the synthesis of 2,4,5-trisubstituted imidazoles by a one-pot condensation of benzil derivatives, aryl aldehydes and ammonium acetate in EtOH.