Understanding the coupling between magnetism and ferroelectricity is of high fundamental and technological importance. [1][2][3][4][5] For example, a sufficiently strong coupling between magnetic and dielectric properties may enable switching of the magnetization by means of an electric field, thereby drastically reducing the thermal power needed for a magnetic memory. If electric writing and magnetic reading were to be used, one of the layers in spin valves composed of ferromagnetic and magnetoelectric layers would no longer have to be pinned. [6] Giant magnetoelectric materials facilitate highly efficient elastic interactions and a strong magnetic response to an electric field (or vice versa) via magnetostriction and piezoelectric effects. [7,8] Several materials possess both ferroelectricity and a co-operative magnetism; however, the coupling between these properties is not necessarily large. The structural and electronic circumstances that would favor a large coupling remain unexplored, partly due to the lack of materials with a large coupling. Here we report that such a large coupling occurs in BiCoO 3 , for which an external electric field can induce a strong magnetic response by changing the spin-state of cobalt from a magnetic high spin (HS) state to a nonmagnetic low spin (LS) state. The simultaneous presence of strong electron-electron interaction within the transition metal d manifold and a sizable hopping interaction strength between the transition metal d and oxygen p states are primarily responsible for a wide range of properties exhibited by perovskite-like oxides. Several ferroelectric perovskites undergo a phase transition from a high-temperature, high-symmetry phase that behaves as an ordinary dielectric to a spontaneously polarized phase at low temperature. Considerable research activities are focused on understanding the nature of and the driving force for such ferroelectric transitions. The electric and magnetic properties of cobaltites depend on the spin state of the Co ions, that is, whether they are in LS, intermediate spin (IS), or HS states (simplified pure ionic limit). For example, LaCoO 3 is a diamagnetic insulator at low temperature and transforms to the paramagnetic state at 90 K due to an LS-IS transition. [9,10] Metamagnetism from spin-state transitions may give rise to exciting phenomena such as giant magnetoresistance, [11] giant magnetocaloric effect, [12] shape memory effect, [13] etc. We show presently that metamagnetism can also lead to giant magnetoelectric coupling. Generally, spin-state transitions are induced by hole/electron doping, temperature, magnetic field, pressure, and/or lattice strain. For the first time we here show that spin-state transitions can also be induced by an electric field in the case of magnetoelectric materials that display magnetic instabilities. Materials with pure ionic bonding typically possess centrosymmetric structures owing to the minimizing of short-range Coulomb repulsions and they are hence nonferroelectric. The noncentrosymmetry required...