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In this paper, a bimetallic Metal-Organic Framework (MOF) CoNiBTC was employed as a precursor for the fabrication of bimetallic nanoalloys CoNi@C evenly disseminated in carbon shells. These functional nanomaterials are characterized by powdered X-ray diffraction (PXRD), Fourier Transform Infra-Red spectroscopy (FTIR), surface area porosity analyzer, X-ray photoelectron spectroscopy (XPS), Field emission scanning electron microscopy (FESEM), Transmission electron microscopy (TEM), Hydrogen Temperature-Programmed Reduction (H₂ TPR), CO₂ Temperature-Programmed Desorption (CO₂-TPD), and Inductively Coupled Plasma Mass Spectrometry (ICP-MS). This nanocatalyst was utilized in the synthesis of benzimidazole from <i>o</i>-phenylenediamine in the presence of CO₂ and H₂ in a good yield of 81%. The catalyst was also efficient in the manufacture of several substituted benzimidazoles with high yield. Due to the existence of a bimetallic nanoalloy of Co and Ni, this catalyst was also employed in the methanation of CO₂ with high selectivity (99.7%).