► At the resonance frequency, α E,A in the axial mode increases linearly even though H DC > 8000 Oe. ► The maximum of α E,V in the vertical mode with H DC = 270 Oe is much higher than that with H DC = 7000 Oe. ► The ME voltage coefficient increases with cylinder diameter. ► The resonance frequency of cylindrical layered composites decreases with increasing cylinder diameter. Magnetoelectric (ME) Ni–PZT–Ni cylindrical layered composites have been prepared by electroless deposition. The ME effect was measured by applying both constant and alternating magnetic fields parallel and perpendicular to the cylinder axis direction. The ME voltage coefficient increases with cylinder diameter. Both experimental and calculated data indicate that the resonance frequency of Ni–PZT–Ni cylindrical layered composites decreases with increasing cylinder diameter. We can apply this characteristic of resonance frequency to design a kind of ME composites with the controllable resonance ME coupling.