In this project, we tried to synthesis derivatives of 4-(benzylidene) aminopyrimidine (I), (benzo[d]thiazol-2-ylimino) methylphenol (II), n-benzylideneazine (III) and n-benzylideneaniline (IV) with natural catalyst and solvent instead of chemical catalyst and solvent condition as green chemistry. The advantages of the use of natural catalyst without organic solvent are eco-friendly, affordable, very safe and easy reaction conditions. The synthesized product was characterized by melting point, IR, 1H NMR and 13C NMR spectra. All derivatives of 4-(benzylidene)aminopyrimidine (I) were tested against gram-positive and gram-negative bacteria by minimum inhibitory concentration (MIC) and disk diffusion methods for antibacterial activities.