© 2023, King Fahd University of Petroleum & Minerals.The effect of zirconium (Zr) substitution in nickel–cobalt ferrites, Co0.5Ni0.5ZrxFe2−xO4 (0.0 ≤ x ≤ 1.0) produced by the hydrothermal method on the electrical, magnetic, microstructural and characteristic properties are reported. A secondary phase as tetragonal-ZrO2 phase in the crystal system is detected and have both M-type hexagonal and tetragonal nanocrystallites between 32 and 67 nm. Refined structural parameters using Rietveld analysis are carried out, resulting in lattice parameters, the unit cell volume, parameter ratios, and the crystallite size using the TOPAS refinement program. In addition, residuals for the RBragg factor and goodness of fit (χ2) value for each concentration are represented. The Rietveld analysis determines that the predicted and actual diffraction patterns are in accord. Furthermore, the Zr effect is presented in unit volume as seen by the drop in peak intensity that occurs (with the addition of Zr) due to the lattice tension. Moreover, the morphological analyses indicate that the shape transformed from agglomerated clusters to oval-shaped structures and a reduction in grain size. Fourier transform infrared (FT-IR) analysis in the range of 4000–450 cm−1 correlates with the presence of the hexagonal spinel ferrite structure. The dielectric parameters, such as the relative permittivity, tangent loss, and ac conductivity, are experimentally measured with the oscillation voltage level of 0.05 V in the frequency range of 0.1–10 MHz. The dielectric permittivities and tangent losses of the specimens decreased with an increment in frequency. Magnetic measurements reveal that the values of coercivity (Hc) have the propensity to increase relating to the zirconium concentration.