The reactions of Cu (II), Zn (II) and Cd (II) chloride or bromide with (E)‐1‐(3,4‐dimethoxybenzylidene)‐4‐methylthiosemicarbazone (MTSVT) lead to the formation of new complexes. They were characterized by spectroscopic studies: IR, ¹H and ¹³C NMR. The crystal structures of the compounds [MTSVT] (L), [ZnBr₂(MTSVT)₂] (2), [CdCl₂(MTSVT)₂] (3) and [CdBr₂(MTSVT)₂^.H₂O] (4) were determined by X‐ray diffraction. For complexes 2–4, the ion is coordinated through the sulfur atom. All compounds were tested for their antifungal activity against human pathogenic fungi Candida albicans and Aspergillus fumigatus, and for their antibacterial activity against Gram (+) Bacillus subtilis and Enterococcus faecalis as well as against Gram (−) bacteria such as Paracoccus yeei and Acinetobacter baumanii. The results indicated that the metal complexes exhibited a marked enhancement in antibacterial activity compared with the parent Schiff base.