The novel sandwich composites were prepared by sandwiching a polyvinylidene fluoride/TbDy-Fe alloy composite (PVDF/Terfenol-D) between polyvinylidene fluoride/lead zirconate titanate composites (PVDF/PZT). The maximum magnetoelectric effect voltage coefficient, (dE/dH) 33max , of the sandwich composites is higher than that of three-phase composites at their own optimal loading level of Terfenol-D. This is attributed to less interface relaxations of strain and better polarization of the sandwich composites. When the volume fraction of Terfenol-D is higher than 0.10, no coupling interaction for three-phase composites could be observed, but (dE/dH) 33max of sandwiched composites still reached 20 mV/(cm•Oe). At high magnetic field intensity, the magnetoelectric effect voltage coefficient, (dE/dH) 33 , of sandwich composites is higher than that of three-phase composites; at low magnetic field intensity, (dE/dH) 33 of sandwich composites is lower than that of three-phase composites. At their resonance frequency, the (dE/dH) 33max of the sandwich composites and the three phase composites are 150 mV/(cm•Oe) and 42 mV/(cm•Oe), respectively. This significant increase of (dE/ dH) 33max at resonance frequency confirms the improvement of maximum magnetoelectric effect coefficient via sandwich-structured composites.