Electric field (E-field) tunable multiferroic devices such as tunable RF devices and memory storage mediums require strong magnetoelectric interactions. In this paper, we demonstrated a Terfenol-D/lead zinc niobate-lead titanate composite bilayer structure with an E-field-induced magnetic anisotropy field of 3500 Oe and a magnetoelectric coefficient of 580 Oe cm/kV. This is the largest E-field induced anisotropy reported to date, resulting in a strong dependence of magnetization process and tunable ferromagnetic resonance in both amorphous and crystalline Terfenol-D films. In addition, the magnetostriction constants of crystalline and amorphous Terfenol-D were estimated to be 420 ppm and 320 ppm, respectively, which are close to report values. Electrically manipulating magnetic performance holds great potential for future ultra-low power, lightweight, tunable magnetic devices, and memory storage.