An electrode-arrayed magnetoelectric (ME) composite was proposed, in which the positive and negative electrodes of the PZT-5H plate (Pb(Zr0.52Ti0.48)O3) were equally divided into a 2 × 5 array, while the PZT plate remained intact. The ME voltage coefficients of these 10 sections were measured individually and in parallel/series modes. The magnetoelectric coefficient is doubled compared with un-arrayed condition, when the 10 sections are connected in parallel/series using an optimized connecting sequence derived from the charge matching rule. This scheme can also be applied to other types of layered magnetoelectric composites to obtain additional magnetoelectric effect from the original composite structure.