A method of manufacturing a magnetoelectric composite material having a 0-3 type connectivity is provided. The manufacturing method includes manufacturing a slurry including an alignment material including one material selected from among a magnetostrictive material and a piezoelectric material. The slurry further comprises a seed composition comprising the other material from the magnetostrictive material and the piezoelectric material. The method further comprises molding the manufactured slurry to manufacture a molding material, and plasticizing and firing the molding material.