Disclosed is a magnetoelectric (ME) composite including both a piezoelectric material and a magnetostrictive material, wherein a piezoelectric single crystal material having high piezoelectric properties is used as the piezoelectric material, and a metal magnetostrictive material having high magnetostrictive properties is used as the magnetostrictive material, thus achieving an ME composite having a layered structure via adhesion. When the ME layered composite is manufactured such that a crystal orientation of the piezoelectric single crystal material is set to a thickness direction, high ME voltage coefficient, which is at least doubled, compared to a conventional crystal orientation, can be obtained, and such an effect is further maximized in the resonance of the composite.