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Series of 1-benzoyl-4-arylthiosemicarbazides were efficiently synthesized and evaluated for their antibacterial activities. The results indicated that most of the compounds possessed activity against the Gram-positive bacterial species. Some structural and electronic parameters have been determined to explore the correlation between the biological activity and structure. The molecular study suggests that inhibitory action of studied thiosemicarbazides towards Gram-positive bacterial species is connected with electronic parameters rather than the geometry of the molecule.