Using aerosol deposition, 2-2 layered structured magnetoelectric (ME) composites were fabricated. Almost fully dense, polycrystalline Pb(Zr,Ti)O3-based piezoelectric thick films with thickness of over 20 similar to mu m were fabricated on the sintered CoFe2O4 (CFO) magnetostrictive ceramics. Although the sintered CFO ceramics were not fully dense, the aerosol deposited piezoelectric films showed good adhesion and there were no noticeable cracks. The piezoelectric films thus obtained showed not only dielectric, ferroelectric, and piezoelectric properties, but also superior ME characteristics with a voltage coefficient of over 130 similar to mV/cm.Oe, especially the PZTPZN films.