Abstract: CoFe₂O₄ powders of spinel structure and BaTiO₃ powders of perovskite structure were prepared using solid phase synthesis. Then the powders were mixed in the molar ratio of 2:8. The different sintering aids were added. The effect of additive on composition microstructure, dielectric properties, ferroelectric properties and magnetic properties of CoFe₂O₄/BaTiO₃ multiphase magnetoelectric material were studied. The results show that it is difficult to achieve the purpose of sintering densification when only Bi₂O₃ is added; when sintering aids containing CaCO₃-SiO₂, the sintering performance of CoFe₂O₄/BaTiO₃ multiphase magnetoelectric material is improved. At the same sintering temperature, the density of CoFe₂O₄/BaTiO₃ multiphase magnetoelectric material is improved, and the dielectric properties, ferroelectric and magnetic properties are optimized for a certain degree.