A new series of 1-((1-(1H-benzo[d]imidazol-2-yl)ethylidene)amino)-6-((arylidene)amino)-2-oxo-4-phenyl-1,2-dihydropyridine-3,5-dicarbonitriles (4a-o) have been synthesized for the development of antimicrobial agents. Newly synthesized compounds were evaluated for their in vitro antibacterial activity against Gram-positive bacteria (Pseudomonas aeruginosa, Streptococcus pyogenes), Gram-negative bacteria (Escherichia coli, Staphylococcus aureus), and antifungal activity (Candida albicans, Aspergillus niger, Aspergillus clavatus). These compounds were characterized by infrared, H-1 NMR, C-13 NMR, and mass spectra. The synthesized compounds 4b, 4e, 4h, and 4k showed potent antimicrobial activity against tested microorganisms.