| Summary: | A series of Schiff base derivatives, namely <i>N</i>-(4-methoxyphenyl)-1-(1-methylbenzimidazol-2-yl)methanimine (L<sup>1</sup>), 4-methoxy-<i>N</i>-[(1-methylbenzimidazol-2-yl)methyl]aniline (L<sup>2</sup>), and 2-[(<i>E</i>)-(1-propylbenzimidazol-2-yl)iminomethyl]phenol (L<sup>3</sup>), were synthesized. These compounds feature different linker groups, including –CH=N–, –CH<sub>2</sub>–NH–, and –N=CH–, respectively. During the process of zinc(II) and cadmium(II) complexation in the presence of the <i>closo</i>-dodecaborate [B<sub>12</sub>H<sub>12</sub>]<sup>2–</sup> anion, it was observed that ligand L<sup>3</sup> underwent degradation. Consequently, two compounds were isolated, [Zn(Bz-NH<sub>2</sub>)<sub>2</sub>(CH<sub>3</sub>COO)<sub>2</sub>] and (HBz-NH<sub>2</sub>)<sub>2</sub>[B<sub>12</sub>H<sub>12</sub>]∙2CH<sub>3</sub>CN, both containing 1-propyl-2-aminobenzimidazole (Bz-NH<sub>2</sub>), which is a degraded fragment of the ligand. Several new zinc(II) and cadmium(II) coordination compounds were synthesized and characterized using various physicochemical analysis methods, including elemental analysis, IR, and UV spectroscopy. Additionally, X-ray diffraction and Hirshfeld surface analysis were performed for compounds [Cd(L<sup>2</sup>)<sub>2</sub>(CH<sub>3</sub>CN)(H<sub>2</sub>O)][B<sub>12</sub>H<sub>12</sub>], [Zn(Bz-NH<sub>2</sub>)<sub>2</sub>(CH<sub>3</sub>COO)<sub>2</sub>], and (HBz-NH<sub>2</sub>)<sub>2</sub>[B<sub>12</sub>H<sub>12</sub>]∙2CH<sub>3</sub>CN, as well as for ligand L<sup>2</sup>.
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