In order to obtain additional microstructural information on the Co n MoS(1-5) cluster and establish a theoretical foundation for subsequent investigations of its electronic properties and catalytic performance, this study investigates the atomic interaction relationships and frontier orbital compositions of the cluster. To accomplish this,we utilized density functional theory with the B3LYP functional and def2-TZVP basis set to optimize the cluster configuration and perform theoretical analysis under various spin multiplicities with the Gaussian09 software package.The results demonstrate the existence of 21 stable configurations. We employed theoretical analyses of the AIM theory,electron localization function, and deformation density to obtain information on the degree of internal interaction and electron density transfer trends of the cluster. Our findings indicate that covalent bonding interactions between Co, Mo,and S atoms are strong in the internal atom interaction of the cluster, with S atoms exhibiting high localization and low probability of electron escape from the domain. In contrast, Co and Mo atoms exhibit strong delocalization and are likely to exchange electrons with the outside. Through Hirshfeld analysis of atomic contribution rates, we observed that metal atoms are the primary contributors to the HOMO and LUMO orbitals, with Mo and Co atoms dominating the frontier orbitals. Overall, we conclude that covalent bonding is the primary atomic interaction within the cluster, but the strength of these interactions varies. Mo and Co atoms should be the focus in chemical reactions of the cluster.