The (Bi4Ti3O12)0.4–(CaCu3Ti4O12)0.6{(BTO)0.4–(CCTO)0.6} nanocomposite was fabricated in powder, thin film, and thick film configurations employing sol-gel, spin coating, and screen printing techniques. The weight loss observed in TGA and the presence of an exothermic peak in the DTA results confirm that 900°C is the optimal temperature for preparing a high-purity dual-phase composite. The XRD patterns and phase fraction analysis substantiate the formation of distinct orthorhombic structured BTO and cubic structured CCTO phases. FESEM images depict an irregular shape, dense microstructure with minimal pores, and a bimodal distribution. The EDAX results provide direct evidence of the formation of nanocomposites according to the stoichiometric ratio. The confirmation of good compatibility between both constituent phases is affirmed by the observation of vibration modes in the Raman spectra. The nanocomposite thin film demonstrates superior dielectric properties (with a dielectric constant of approximately 3534 and a lower dielectric loss of about 2.41), as well as optimal ferroelectric properties (including a remnant polarization of around 12.37 µC/cm2 and coercivity of approximately 0.95 kV/cm) compared to its powder and thick film counterparts. These observed characteristics of (BTO)0.4–(CCTO)0.6 nanocomposite materials strongly correlate with their practical suitability for use in technologically advanced microwave and microelectronic devices.