A series of streptocide-, sulfacyl-, norsulfazole-, ethazole-, sulfadimezine-, and sulfapyridazine-containing copper(II) and nickel(II) salicylidenethiosemicarbazidates and salicylidene-4-phenilthiosemicarbazidates possessing high antimicrobial activity has been synthesized. The composition and probable structures of the obtained coordination compounds are proposed based on elemental analysis and magnetochemical, IR spectroscopy, and thermogravimetric data. The dependence of the antimicrobial activity of compounds on the nature of the central atom, sulfanilamide, and phenyl radicals in the thiosemicarbazide fragment of azomethine has been studied with respect to ten species of staphylococcus, streptococcus, and intestine bacillus strains. The maximum activity was exhibited by norsulfazole-and sulfacyl-containing Cu(II) salicylidenethiosemicarbazidate and Cu(II) salicylidene-4-phenilthiosemicarbazidate.