The effect of cosintering time on magnetoelectric (ME) behavior of Sr, La doped lead zirconate titanate multilayer–nickel zinc ferrite composites fabricated by the tape-casting method has been investigated. Powders of individual phases, viz., Pb(1 − x − 3y/2)SrxLay(Zrz,Ti(1 − z))O3 (PSLZT) and Ni0.6Zn0.4Fe2O4 (NZFO), were prepared by the solid-state reaction method, and their respective thick films were fabricated by the tape-casting method. A PSLZT multilayer having Pt inner electrodes stacked onto NZFO laminated composites was cosintered at 1060 °C for 1–10 h. Cosintered, warpage-free, and delamination-free layered composite thick film structures were analyzed by scanning electron microscopy. Microstructure at the interface could be crucial for better magnetoelectric coupling, and, hence, the microstructure of the interface was analyzed as a function of sintering time at a fixed sintering temperature. Elemental mapping revealed a negligible interdiffusion between PSLZT and NZFO phases. Composites cosintered for different time durations were analyzed for their ferroelectric behavior. Further, impedance spectrum analysis indicated clear resonance behavior for the composites cosintered for 2 and 6 h. All the composites were analyzed for magnetoelectric properties at different applied DC magnetic fields having a superimposed ac magnetic field of a fixed frequency and different ac frequencies at fixed DC magnetic fields. The magnetoelectric coefficient was found to increase with an increase in the sintering time of up to 6 h and an ME coefficient of 230 mV/cm Oe with a self-bias nature. Magnetoelectric resonance behavior was also studied, which showed an ME voltage coefficient of 6 V/cm Oe for composites sintered for 6 h at resonance.

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