A series of novel composites with the composition of xNiCuZn-(1-x)PZT (NiCuZn: Ni0.2Cu0.2Zn0.6Fe2O4; PZT: PbZr0.52Ti0.48O3.) were prepared by solid-state reaction methods. The presence of ferromagnetic NiCuZn ferrite phase and ferroelectric PZT phase was confirmed by XRD analysis. It was revealed that composite materials exhibit typical ferromagnetic hysteresis behaviors. With the increase of phase fraction of NiCuZn ferrite, the permeability of composites increases and the natural resonance peak appears. Meanwhile, the maximum of quality factors shifts to the lower frequency.