<p>Two bimetallic organic complexes were prepared through a hydrothermal synthesis route, employing 2-(2-pyridyl)benzimidazole as the ligand along with soluble salts of molybdenum, cobalt, and copper as metal precursors. The obtained compounds were determined to have the molecular formulas C₇₂Co₂Mo₈N₁₈O₂₉H₆₀ and C₁₂H₁₁CuMo₂N₃O₇. Their structural, morphological, and elemental oxidation state characteristics were systematically analyzed using single-crystal X-ray diffraction, powder X-ray diffraction, scanning electron microscopy, and X-ray photoelectron spectroscopy. Electrochemical assessments revealed that both complexes exhibit promising performance as electrode materials for supercapacitors and lithium-ion batteries. Notably, the MoCo-based complex outperformed the other in both aqueous and organic electrolytes. To gain further insight into the origin of this enhanced performance, first-principles calculations were carried out. The results indicated that although the band gaps of the two materials are similar, MoCo possesses a higher density of energy states near the Fermi level, implying a greater number of available ion transport channels. These results provide valuable guidance for the design of high-performance electrode materials for energy storage applications.</p>