Particulate ceramic-composite (1 − x) BaTiO3 + x NiFe2O4 with compositions (x = 0.2, 0.4, 0.6, and 0.8) was prepared by solid-state synthesis. The presence of two phases (spinel and tetragonal) in the hybrid composite was confirmed by the XRD. Quantitative phase analysis with structural refinement was carried out using a profile refinement method. The variation of the capacitance with frequency was studied and for x = 0.6, the graph shows a maximum capacitance of 258 pF at 100 Hz. The saturation magnetization (Ms) calculated from the magnetic hysteresis measurement increased with increase in the ferrite content and reached a maximum of 23.282 emu/g for x = 0.8. The material’s microstructure particle sizes varied from 1.74 μm to 3.27 μm as shown by SEM micrographs. Electron density analysis was used to study the bonding between the atoms of the composite (1 − x) BaTiO3 + x NiFe2O4 with compositions (x = 0.2, 0.4, 0.6, and 0.8). This is a new approach to studying the electron distribution and bonding nature of the samples. The analysis confirmed that the bonds of the individual atoms were responsible for the electric and the magnetic properties of the prepared ceramic composite.