The generation of spin-based multi-qubit entangled states in the presence of an electric field is one of the most challenging tasks in current quantum-computing research. Such examples are still elusive. By using non-equilibrium Green′s function-based quantum-transport calculations in combination with non-collinear spin density functional theory, we report that an eight-spin-qubit entangled state can be generated with the high-spin state of a dinuclear Fe(II) complex when the system is placed in a molecular break junction. The possible gate operation scheme, gating time, and decoherence issues have been carefully addressed. Furthermore, our calculations reveal that the preservation of the high spin state of this complex is possible if the experimentalists keep the electric-field strength below 0.78 V nm−1. In brief, the present study offers a unique way to realize the first example of a multi-qubit entangled state by electrical means only.