CoFe2O4-Pb(Zr0.52Ti0.48)O-3 (CFO-PZT) multilayered composite film was prepared on Pt/Ti/SiO2/Si substrate via a sol-gel method and spin-coating technique. Results show that PZT and CFO phases exist in the composite film, calcined at 700 A degrees C, besides substrate phase, and no obvious impurity phases can be detected. The composite film exhibits layered structure with obvious boundary between CFO and PZT films. Ferroelectric and ferromagnetic properties were simultaneously observed in the composite film, evidencing the ferroelectric and ferromagnetic properties in the composite film. The composite film exhibits both good magnetic and electric properties, as well as, magnetoelectric (ME) effect. The saturation magnetization value of the composite film is lower than that of the pure CFO film derived by the same processing as a result of the effect of the nonferromagnetic PZT layers. Ferroelectric hysteresis loops reveal that saturated polarization and remanent polarization of the composite film are lower than those of the pure PZT films. The composite film exhibits a very large ME effect, which makes the composite film attractive for technological applications as devices.