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High‐dielectric constant (high‐K) polymer nanocomposites based on nematic liquid crystals and CaCu₃Ti₄O₁₂ (CCTO) nanoparticles have been prepared. The host matrix is polymer dispersed liquid crystals (PDLC) in which LC (E7) droplets are dispersed in different polymer blends ratios of poly vinyl chloride/poly aniline (PVC/PANI). The PDLC (PVC/PANI/E7) in the appropriated ratios; (90/10/5), (75/25/5), and (50/50/5) were composited with 10 wt% CCTO nanoparticles. The IR spectra recorded for the PDLC nanocomposites present a spectrum similar to that of pure PDLC but with a slight shift of the peak positions. The addition of PANI and CCTO to PDLC enhances the thermal stability of the nanocomposites. SEM demonstrates agglomerates of CCTO dispersed in the polymer textures. Moreover, the addition of E7 facilitates the integration of PANI in PDLC matrix. The broadband dielectric spectrum shows high …