The magnetoelectric (ME) coupling of cylindrical trilayered composite was studied in this paper. The Ni-lead zirconate titanate (PZT)-Ni trilayered cylindrical composite was synthesized by electro-deposition. The maximum ME voltage coefficient of cylindrical ME composite is 35V/cm Oe, about three times higher than that of the plate trilayered composite with the same raw materials and magnetostrictive- piezoelectric phase thickness ratio. The high ME voltage coefficient of cylindrical composite owes to the self-bound effect of circle. Moreover, the resulting complex condition can induce a double peak in the field dependence of ME coefficient.