Computational investigations employing Density Functional Theory (SMD(benzene)-M06-2X-D3/6-311+G*) predict that stable metal-free mono (Lewis base)-stabilized borylenes could strongly bind with transition metal (Fe and Ni) complexes. The binding results in increase in the Lewis basicity of the metal centers thus facilitating the formation of metal only Lewis pairs (MOLPs) of the form [L(CO)4Fe → GaCl3] and [L(CO)3Ni → GaCl3] (L = electron donating ligands). Further, the binding of different ligands with the metals as well as bonding in the MOLPs have been further investigated with the help of QTAIM and EDA-NOCV analyses.