In this letter we present a magnetic field-induced giant phase shift effect under resonant frequency in the bilayered magnetoelectric composite of Tb0.3Dy0.7Fe2(Terfenol-D) and Pb(Zr,Ti)O3. When the bias magnetic field is varied from 0.1 T to 0.3 T, the phase shift of the magnetoelectric effect under 83.2 kHz was as large as 180°, which implies a complete transformation from capacitor behavior to inductor behavior. The phase shift was analyzed in the polar coordinates, and the mechanism of this giant phase shift was considered as the ΔE effect of Terfenol-D. This giant phase shift effect may benefit existing phase modulation techniques.