The rapid development of smart and sophisticated miniaturized electronic devices put a high demand for high permittivity material. In the current report, we analyze structural, morphological, and dielectric response of spinel-perovskite composites consisting of CoFe2O4 (CFO) as the spinel phase and BiFeO3 (BFO) as the perovskites phase. Here pristine BFO and CFO are fabricated using Sol—Gel auto-combustion route and their composites with a recipe (1-x) BiFeO3 - (x) CoFe2O4 (x = 0.0, 0.1, 0.2 and 0.3) using solid-state reaction technique. Structural investigation identifies presence of rhombohedral perovskite phase of BFO and cubic spinel phase of CFO and thus guarantees the formation of the composite. The crystallite size increases from 16 to 36 nm for BFO and 39.5–54 nm for CFO. The distribution of well-shaped particles with a reduction in grain size in range of 50–400 nm is witnessed in morphological analysis with the increment of CFO contents in composites. Elemental purity and the presence of various elements according to their stoichiometric ratio are witnessed during elemental investigation. A detailed analysis of the dielectric permittivity, electric modulus, and impedance of these compositions is carried out to investigate their suitability for electronic and energy storage devices. The nanocomposites under study exhibit a dielectric constant of 1126 at 100 Hz for x = 0.3, which decreases to 102 at 1 MHz. Concurrently, the tangent loss for x = 0.3 is observed to be 3.37 at 100 Hz, decreasing to 0.31 at 1 MHz. However, a decrease in dielectric loss and increase in impedance is noticed when the concentration of CFO in BFO nano-composite is increased which reflects the reduction in power losses and better control in electronic conductivity and thus highlights the role of these compositions for advanced energy storage electronic devices.