ABSTRACT In this work, we investigate how the preformed microstructure and field‐induced particles' mobility in magnetoactive elastomers (MAE) influence magnetoelectric coupling in two‐layer structures composed of a piezoelectric polymer (PEP) film and a MAE layer. In anisotropic MAE, iron microparticles are pre‐aligned into chains oriented perpendicular to the sample plane, defining the magnetic “easy axis.” The structural anisotropy enhances the resonance mechanical deformation of the MAE laye