Syntheses, structures, and antimicrobial activities of cobalt(III) complexes with two tetradentate Schiff-base ligands, (BA) 2 en ¼ bis(benzoylacetone)ethylenediimine dianion and (acac) 2 en ¼ bis(acetylacetone)ethylenediimine dianion, and two axial pyridines (py) have been investigated. These complexes were characterized by FT-IR, 1 H-NMR, UV-Vis spectroscopy, and elemental analysis. The crystal structures of the complexes were determined by X-ray crystallography. Single-crystal X-ray diffraction analyses revealed that both complexes have distorted octahedral environments, Schiff-base ligand coordinates cobalt in four equatorial positions, and the two axial positions are occupied by pyridines. The pyridines and Schiff-base ligands are involved in N-HÁ Á ÁO hydrogen bonds with perchlorate. Biological activities of the ligands and metal complexes have been studied on Staphylococcus aureus, Escherichia coli, and Bacillus subtilis by the well diffusion method. The activity data show the metal complexes to be more potent than the parent ligand against two bacterial species.