0-3 type magnetoelectric(ME) composites of PbTiO3(PT) and CoFe2O4(CFO) were prepared by a conventional solid-state reaction method with different volume fraction. The composites exhibited ferroelectric phase and ferromagnetic phase coexisting. The ferroelectric and magnetic properties of as-sintered samples were measured. The magnetic properties change regularly with the test frequency. But the dielectric permittivity shows the anomalies, which can be attributed to constraints and dilutions from the ferromagnetic phase and the element diffusion.