Aseries of copper (II) streptocide-, sulfacyl-, norsulfazole-, ethazole-, and sulfadimezine-containing naphthalidenethiosemicarbazidates and napthalidene-4-phenylthiosemicarbazidates with high levels of antimicrobial activity were synthesized. Elemental analysis, magnetochemical, IR spectroscopic, and thermogravimetric data were used to confirm the compositions and structures of the resulting complexes. The effects of the nature of the central atom and the influences of the sulfanilamide and phenyl radicals in the azomethine thiosemicarbazone fragment on the antimicrobial activity of the compounds against 10 strains of Gram positive and Gram negative microorganisms were studied. The most active of the compounds synthesized were the copper norsulfazole-, ethazole-, and sulfadimezine-containing naphthalidenethiosemicarbazidates.