A thick film of P(VDF-TrFE) piezoelectric polymer and a 48%nickel-iron (48%NiFe) alloy is employed to form a magnetoelectric (ME) layered composite to attain a ME coupling coefficient
α
ME
as high as 1002 mV cm−1 Oe−1. Theoretical analysis indicates a significant strain transfer of close to 79%. Compared with P(VDF-TrFE)/nickel bilayer laminate composite, 48%NiFe alloy shows an enhancement of
α
ME
by 53% due to the high piezomagnetic coefficient. Additionally, finite element methodology simulation using COMSOL® Multiphysics is used to corroborate the experimental results and theoretical estimates. The energy harvesting application is demonstrated by measuring the voltage from the laminate composite atop a small cooling fan, which produces a peak-to-peak ac voltage of 0.868 V. Comparative analysis with P(VDF-TrFE)/nickel bilayer laminate this value is 54% higher proving that the developed laminate composite is an efficient ME based energy harvester.