Zinc substituted nickel-cobalt ferrites, i.e., ZnxNi0.8−xCo0.2Fe2O4 (x=0.0, 0.05, 0.10 and 0.20) with average crystallite size 100 nm were synthesized by citrate-gel auto-combustion method to investigate effects of Zn2+ substitution on the structural and dielectric properties. Both X-ray diffraction (XRD) and IR spectroscopy studies confirms the formation of pure cubic spinel structure. Variation of lattice parameter infers Vegard’s law linear dependence with the addition of Zn2+ concentration. The temperature-dependent behavior of dielectric and modulus spectra has been studied within the frequency range 100 Hz-100 kHz for different temperatures between 100K and 400 K. It was concluded that the dielectric responses of ZnxNi0.8−xCo0.2Fe2O4 are found to be frequency dependent and thermally activated. Also, In the Zn doped ferrites variations of dielectric loss (tan δ) and the imaginary part of electric modulus (Mʺ) show the presence of the non-Debye type of dielectric relaxation. Rise in Zinc concentration leads to a decrease in dielectric constant (εr) due to the declining of Fe3+–O–M2+ conducting network (M is Co or Ni). Here, we report a low loss tangent factor of the order of for the sample Ni0.6Zn0.2Co0.2Fe2O4 make this composition suitable for high frequency-applications at room temperature.