A simple hot molding technique was used to prepare the laminated composites consisting of polyvinylidene (PVDF)/Tb Dy Fe alloy (Terfenol D) /lead zirconate (PZT), with PVDF/Terfenol D particulate composite as the upper and lower layers. The influence of volume change of the middle layer Terfenol D on the dielectric coefficient, dielectric loss, piezoelectric coefficient and magneto electric coupling coefficient were discussed. Experimental results demonstrated that when the volume fraction of the Terfenol D was 4% in PVDF/Terfenol D/PZT layer in laminated magneto electric composites, magneto electric coupling coefficient and piezoelectric coefficient could be the best, reaching to 1 118 mV/A and 32.4 pC/N respectively.