Magnetoelectric effects and multiferroic materials are very important both for basic science and for practical applications[1-2].Although several multiferroic materials/heterostructures have been extensively studied,finding strong magnetoelectric couplings for the electric field control of the magnetization remains challenging.Here,a novel interfacial magnetoelectric coupling (▽ · P)(M · L) based on three components (ferroelectric dipole P,magnetic moment M,and antiferromagnetic order L) is analytically formulated.As an extension of carrier-mediated magnetoelectricity,the new coupling is shown to induce an electric-magnetic hysteresis loop,as shown Fig.1(e).Realizations employing BiFeO3 bilayers grown along the[111]axis are proposed,as shown Fig.1(a-d).Without involving magnetic phase transitions,the magnetization orientation can be switched by the carrier modulation driven by the field effect,as confirmed using first-principles calculations[3].