Abstract Terfenol-D/Pb(Zr,Ti)O 3 (PZT) bi-layered thin rectangular composites with varying thickness of PZT layer ( t PZT ) were prepared, and the effect of bias magnetic field ( H dc ) on magnetoelectric voltage coefficient ( α V ) was investigated. Two significant peaks could be observed in α V – H dc curve at 1 kHz when t PZT ⩽ 0.8 mm, and the unique shape was attributed to two components of piezomagnetic coefficient for Terfenol-D, which contributed to magnetoelectric coupling and reached the maximum values under different bias magnetic fields. The magnetoelectric voltage coefficients at resonant frequencies for length and bending vibration modes were also strongly dependent on bias magnetic field, and such dependence indicated the tight relationship but not one-to-one correspondence between the two vibration modes and two components of piezomagnetic coefficient.