The magnetoelectric (ME) coupling of a bilayered Ni-lead zirconate titanate composite structure synthesized by electrodeposition was studied in this paper. The ME voltage coefficient was measured in the range of 1-120 kHz as the bias field is parallel to the axial. The results indicate that an electromechanical resonance appears at 59.9 kHz. The bilayered cylindrical ME composite exhibits a special field dependence of ME coefficient. Either for the resonant state or the nonresonant state, above 1 kOe, the ME voltage coefficient increased linearly with the strengthening of bias field, up to 30 V/cm Oe at 8 kOe. (C) 2008 American Institute of Physics.