Three Ni(II) and Zn(II) complexes [Ni(L1)], [Ni(L2)], and [Zn(L3)(DMSO)] (L1 = 2,3-bis(2-hydroxybenzylideneimino)-2,3-butenedinitrile, L2 = 2,3-bis(2-hydroxy-3-methoxybenzylideneimino)-2,3-butenedinitrile, L3 = 2,3-bis(2-hydroxy-1-naphthylideneimino)-2,3-butenedinitrile) were obtained in DMSO by one-pot syntheses. The complexes were characterized by physicochemical and spectroscopic methods. Also, their solid-state structures were determined by single-crystal X-ray diffraction. The geometries of the Ni(II) and Zn(II) complexes were square planar and square pyramidal, respectively. The complexes were screened in vitro against a fungal species and eight species of bacteria, revealing their antimicrobial activity.