To elucidate the structure information and spectroscopic properties, the ground structures of N 1 ,N 5 -bis[pyridine-2-methylene]-thiocarbohydrazone ligand (L) and their corresponding Zn (II) complex ((H 2 L)ZnCl 2 ) (A) and Ni (II) complex ((H 2 L)NiCl 2 ) (B) are optimized at the M06 method. Two conformers, i.e., cis- or trans-, are considered for every species. The ligand presents almost planar structure; while two metal complexes show distorted tetrahedral structure. Subsequently, the spectroscopic properties are calculated using time-dependent density functional theory (TD-DFT) with the polarized continuum model (PCM). For the ligand L, all UV–vis absorption peaks are originated from (p, π)→π * with a character of intraligand charge-transfer (ILCT). With respect to complex A ((H 2 L)ZnCl 2 ), the lowest-energy absorption peak is correlated with HOMO→LUMO transition, which is ascribed to (p, π)→π * with a mixed ligand–ligand charge-transfer and intraligand charge-transfer (LL/ILCT) character. Compared with complex A, the maximum absorption wavelength of complex B ((H 2 L)NiCl 2 ) exhibits red shift.