The authors fabricated Pb(Zr0.52Ti0.48)O3–NiFe2O4 composite films consisting of randomly dispersed NiFe2O4 nanoparticles in the Pb(Zr0.52Ti0.48)O3 matrix. The structural analysis revealed that the crystal axes of the NiFe2O4 nanoparticles are aligned with those of the ferroelectric matrix. The composite has good ferroelectric and magnetic properties. The authors measured the transverse and longitudinal components of the magnetoelectric voltage coefficient, which supports the postulate that the magnetoelectric effect comes from direct stress coupling between magnetostrictive NiFe2O4 and piezoelectric Pb(Zr0.52Ti0.48)O3 grains.