This paper reports the application of the Ru2+, Cu+, and Fe2+ complexes in form of RuL2(SCN)2, CuL2(SCN)2− for dye-sensitized solar cell (DSSC) development. The calculation results, given by quantum chemistry, demonstrated that the complex containing copper is more suitable than the one containing iron. The modification of Cu(I) complex by using various numbers of ligands enhanced photon absorption capacity as well as the absorption range. The addition of an organic ligand such as an electron attraction group to the benzene ring gave a better result as compared to the inorganic ones. Based on the analysis conducted, CuM2(SCN)2− is considered as potential material for N3 replacement.