The converse magnetoelectric effect resulting from the electric-field-induced motion of 90° domain walls in a ferromagnetic film coupled to a single-domain ferroelectric substrate is described theoretically. To that end, the volume fractions of 90° domains with differently oriented in-plane magnetizations are calculated as a function of in-plane strains using the dislocation modeling of stress sources in polydomain heterostructures. Being combined with piezoelectric deformations of a ferroelectric substrate in an electric field, this yields magnetoelectric susceptibilities of ferromagnetic-ferroelectric composites. Remarkably, a giant magnetoelectric susceptibility about 4 × 10−5 s/m is predicted for hybrids comprising Co40Fe60 films coupled to the Pb(Zn1/3Nb2/3)O3-6%PbTiO3 single crystal.