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Two new salicylaldimine-based N-heterocyclic hydrazone ligands, N'-[(2-hydroxyphenyl) methylene]-2-(2-phenyl-1H-benzimidazol-1-yl)acetohydrazone (H₂L¹) and 2-[2-(3-chlorobenzyl)-1H-benzimidazol-1-yl]-N'-[(2-(hydroxyimino)-1-ethylpropylidene]aceto hydrazone (H₂L²) and their homo-binuclear nickel(II), copper(II) and zinc(II) complexes have been synthesized and their structures were identified by using spectroscopic techniques and elemental analysis. The two ligands in both the solid state and solution state show tautomerism, but their complexes don't show tautomerism due to the deprotonation and metal ion(s) binding the ligand in the enol-imine-enol form. The stoichiometries of the complexes were also confirmed by thermal analysis with formation of the corresponding metal oxides. TD-DFT calculations have also been performed to correlate geometrical parameters with the spectral properties of …