Organometallic sandwich complexes, composed of cyclic hydrocarbon ligands and transition-metal atoms, display unique physical and chemical properties. In this work, the electronic and spin transport properties of one-dimensional (1D) VBz 2 ligand bimetallic sandwich complexes, VBz 2 −TM (TM = Cr, Mn, and Fe), are systematically investigated using density functional theory and nonequilibrium Green's function method. The results show that all the 1D infinite molecular wires [(VBz 2 )TM] ∞ (TM = Cr−Fe) are found to be thermodynamically stable with high binding energies (∼1.0−3.45 eV). In particular, they are predicted to be ferromagnetic half metals. Moreover, the I−V curves exhibit negative differential resistance for one, two, and three VBz 2 −TM wires at TM = Cr, Mn, and Fe, respectively, which is of great significance for certain electronic applications. Our findings strongly suggest that the benzene ligand bimetallic sandwich molecular wires are good candidates for potential electronics and spintronics.