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In order to improve the electromagnetic properties of 0.4PZT+0.6NiCuZn-ferrite composites for suppressing electromagnetic interference (EMI), Co2O3 was introduced. The effects of Co2O3 content on the electromagnetic properties of the composite materials were investigated. It was confirmed the existence of local induced anisotropy caused by ordering of Co2+ ions. Permeability spectra of the composites with different Co2O3 content had been resolved into contributions of domain wall resonance and spin rotation relaxation. The fitting results of permeability dispersion revealed the relationships among domain wall resonance, spin rotation relaxation mechanisms, and local induced anisotropy. This increase in local inducted anisotropy results in a decrease of initial permeability and an increase of Q-factor. Meanwhile, Co2O3 additive can improve the dielectric constant and the loss tangent (tandeltae) by increasing the oxygen vacancy concentration.