Magnetoelectric \(Pb{Zr}_{0.52}{Ti}_{0.48}{O}_{3}-Co{Fe}_{2}{O}_{4}\) composites with different molar fractions ( \(Pb{Zr}_{0.52}{Ti}_{0.48}{O}_{3}/Co{Fe}_{2}{O}_{4}=3:1, 2:1, 1:1,\) and \(1:2\) ) were synthesized using citrate-sol–gel route. X-ray diffraction confirmed the presence of perovskite ( \(Pb{Zr}_{0.52}{Ti}_{0.48}{O}_{3}\) ) and spinel ( \(Co{Fe}_{2}{O}_{4}\) ) structures in the produced composites. Scanning electron microscopy showed a homogeneous mixing of \(Pb{Zr}_{0.52}{Ti}_{0.48}{O}_{3}\) and \(Co{Fe}_{2}{O}_{4}\) grains with dense microstructures. The composites' magnetic and ferroelectric hysteresis loops exhibited multiferroic behaviour. Impedance spectroscopy indicated that the composite's overall resistance ( \({R}_{T}\) ) increases up to a \(1:1\) molar ratio due to better phase connectivity, which improves magnetoelectric (ME) coupling. When the molar ratio was \(1:2\) , the \({R}_{T}\) value dropped, which increased the interface charge carrier leakage and reduced the ME coupling. The composite with an equimolar ratio ( \(1:1\) ) achieved the highest ME coefficient ( \({\alpha }_{ME}\) ) value of 10.53 mV/cm.Oe. This value is 14 times higher than the equimolar composite produced by mixing the \(Pb{Zr}_{0.52}{Ti}_{0.48}{O}_{3}\) and \(Co{Fe}_{2}{O}_{4}\) powders due to its dense microstructure, improved connectivity, highest resistance, and reduced leakage current density, making it optimal for ME device applications.
