This study reports the enhancement of magnetoelectricMagnetoelectric coupling in biphasicBiphasic and ternaryTernary composites of BaFe12O19 ceramics and flexibleFlexible films. Three systems were fabricated using different methods: single-phase BaFe12O19 via sol-gel, biphasicBiphasic Na0.5Bi0.5TiO3–BaFe12O19 via solid-state, and ternaryTernary PVDFPolyvinylidene fluoride (PVDF) – Na0.5Bi0.5TiO3–BaFe12O19 via solution casting. The structural and morphological studies were performed using an X-ray Diffractometer and Scanning Electron Microscope which showed successful formation of the phases in the three systems. DielectricDielectrics properties investigated at room temperature showed the dominance of interfacial polarization at lower frequencies. The dielectricDielectrics constant was found to be highest in the biphasicBiphasic composite resulting from the large difference in the resistivity of the constituent phases, while the lowest was observed in the ternaryTernary system due to the dominance of the PVDFPolyvinylidene fluoride (PVDF) polymer. The room temperature multiferroic property of the studied systems was confirmed from the P-E and M-H loop measurements. Furthermore, magnetoelectricMagnetoelectric interaction was analyzed which showed the single phase BaFe12O19 to have a small ME coupling value of ~0.439 mV/cmOe. In comparison, the biphasicBiphasic composite had a higher value of ~26.12 mV/cmOe. This was found to be greatly enhanced up to ~562 mV/cmOe in the ternaryTernary polymer film which can be attributed to better connectivity between the different phases. The polymer film was subjected to a finger-tapping force to investigate the energy harvestingEnergy harvesting property, and an open circuit voltage of about 11.3 V could be observed. With further engineering and better design, the fabricated composite materialComposite material appears to have a bright future in magnetoelectricMagnetoelectric sensorsSensors, pressure sensorsSensors, and mechanical energy harvestersEnergy harvester.