Cerium (Ce3+) substituted Ni-Co ferrites with composition Ni0.3Co0.7CexFe2−xO4 (x = 0.0–0.20, with step size 0.05) were synthesized by sol-gel method. Face-centered cubic (FCC) spinel structure was revealed by X-ray analysis. The crystalline size was calculated ranging between 17.1 and 18.8 nm, lattice constant showed a decreasing trend with increase of Ce3+ contents, furthermore, X-ray density was calculated between 5.30 and 5.69 g/cm3. The two characteristic spinel ferrites absorption bands were seen around 550 (cm−1) and 415 (cm−1) in Fourier transform infra-red (FTIR) spectroscopy. The microstructural and elemental studies were carried out by field emission transmission electron microscopy (FE-TEM) and energy dispersive X-ray (EDX) respectively, the average particle size was calculated around 21.83 nm. Magnetic studies were performed by vibrating sample magnetometer (VSM), which showed that saturation magnetization Ms and remanence Mr decreased with substitution up to x = 0.10 due to small magnetic moment of Ce3+ than Fe3+. The coercivity Hc increased with substitution up to 908.93 Oe at x = 0.05, then it decreased following the trend of anisotropy constant. The dielectric studies exhibited decrease in dielectric parameters with frequency due to decreasing polarization in material. The dielectric loss was significantly decreased in material at high frequency. The Cole-Cole interpretation exhibited conduction mechanism being caused by grain boundary density. These attributes of Ce3+ substituted Ni-Co ferrites suggest their possible use in memory storage, switching and high frequency devices like antenna and satellite systems.