The effect of height on performance of the PZT/Ni cylindrical bilayered magnetoelectric (ME) composites was studied in situ in this paper. Multiple resonant peaks appear between 1 and 300 kHz frequency for cylinders of different heights. The first resonance frequency does not change with the cylinder height decreasing, but the second and the third resonant frequencies increase. The first three resonant modes are attributed to the cylinder radial, first-order height resonance, and second-order height resonance, respectively. The appropriate size and resonance frequency were chosen to obtain the highest ME voltage coefficient when designing cylindrical bilayered magnetoelectric devices. This article provides reference to design cylindrical magnetoelectric devices.