Multilayered multiferroic nanocomposite films of Pb(Zr0.52Ti0.48)O-3 (PZT) and Co0.9Zn0.1Fe2O4 (CZFO) are prepared on general Pt/Ti/SiO2/Si substrates via a simple solution-processing method. Structural characterization by X-ray diffraction and electron microscopy techniques reveals good surface and cross-sectional morphologies of these multilayered thin films. In particular, at room temperature strong ferroelectric and ferromagnetic responses are simultaneously observed in the multilayered thin films, depending on the deposited sequences and volume fractions of ferroelectric PZT phase and magnetic CZFO phase.