Using the auto combustion flash method, Ni1−x+2Mgx+2Fe2+3O4 (x = 0, 0.2, 0.6, 0.8 and 1) nano-ferrites were synthesized. All samples were thermally treated at 973 K for 3 h. The structural analysis for the synthesized samples was performed using XRD, high-resolution transmission electron microscopy (HRTEM), and FTIR. Scanning electron microscopy (SEM) was undertaken to explore the surface morphology of all the samples. The thermal stability of these samples was investigated using thermogravimetric analysis (TGA). XRD data show the presence of a single spinel phase for all the prepared samples. The intensity of the principal peak of the spinel phase decreases as Mg content increases, showing that Mg delays crystallinity. The Mg content raised the average grain size (D) from 0.084 μm to 0.1365 μm. TGA shows two stages of weight loss variation. The vibrating sample magnetometer (VSM) measurement shows that magnetic parameters, such as initial permeability (μi) and saturation magnetization (Ms), decay with rising Mg content. The permeability and magnetic anisotropy at different frequencies and temperatures were studied to show the samples’ magnetic behavior and determine the Curie temperature (TC), which depends on the internal structure. The electrical resistivity behavior shows the semi-conductivity trend of the samples. Finally, the dielectric constant increases sharply at high temperatures, explained by the increased mobility of charge carriers, and decreases with increasing frequency.