Department of Chemistry, Institute of Natural Sciences, University of Gujrat, Gujrat 50700, Pakistan The surfactant assisted co-precipitation method has been used to synthesize the Co2+ and Ni2+ substituted magnesium nanoferrites. The Co2+ and Ni2+ ions substitute the Mg2+ and Fe3+ ions from the magnesium ferrites, respectively. To study the effect of substituted ion concentrations on the dielectric performance of the MgFe2O4 spinel ferrites. The substituted magnesium nanoferrites with the compositions Mg1-x Cox NiyFe2-yO4 (x, y = 0.0, 0.1, 0.2, 0.3, 0.4, and 0.5) were synthesized to notice the effect of substituted ions concentration on the dielectric properties. Thermogravimetric analysis of the precursor precipitates was taken to investigate the stable spinel phase formation temperature. The X-ray diffraction analysis of the all substituted samples confirms the successful formation of the stable spinel phase and also exposes the effects of substituted ions on the crystal structure and unit cell constants. The presence of a characteristic absorption band (400 cm−1, 550 cm−1) of spinel ferrites in the Fourier Transform Infra Red (FT-IR) spectrum of substituted magnesium nanoferrites also confirms the formation of desire phase. The effect of temperature on the conductivity of the all substituted samples was observed within the temperature range of 25°C–300°C by two-probe direct current electrical resistivity measurements. Dielectric measurements of the substituted magnesium nanoferrites were carried out to study their magnetic behavior. The inverse relation of the dielectric parameters of the all substituted magnesium nanoferrites with frequency shows their excellent potential for devices that operate at higher frequencies.Department of Chemistry, University of Okara, Renala Khurd, Okara, Pakistan Department of Chemistry, Allama Iqbal Open University, H-8, Islamabad 45320, Pakistan.