Ferroelectric Pb(ZrZr)O (PZT) and ferromagnetic CoFeO (CFO) composite ceramics, [(1∈-∈x)PZT∈-∈xCFO for x∈=∈10, 20, 30, 40 and 50 wt.%], were prepared by a conventional solid-state reaction method. X-ray diffraction studies revealed that only PZT and CFO phases were present in the composite samples and no other phase was detected. The 0.9PZT-0.1CFO composite ceramic displayed better piezoelectric properties. The piezoelectric resonance frequency increased with the CFO content, but the resonance peak attenuated rapidly and disappeared when the CFO content equaled to 0.5. The permittivity peak temperature was the same as that of pure PZT ceramics. 0.9PZT-0.1CFO composite also had the highest magnetoelectric (ME) coupling coefficient among the studied PZT-CFO composite ceramics. The ME coefficient linearly increased with ac frequency up to 100 kHz. © 2007 Springer Science+Business Media, LLC.