(1-x) (Al0.2La0.8TiO3) + (x) (BiZnFeO3) (x = 0.2 - 0.8) [ALTBZFO] nanocomposites were synthesized via hydrothermal method. The X-ray diffraction patterns indicated the phase transformation from tetragonal to cubic for x = 0.2 to 0.4 - 0.8 samples, respectively. The surface morphology showed the existence of nanospheres like structures. At 1 MHz frequency also, the dielectric constant was increased from 230 to 710 for x = 0.2 – 0.6 samples, respectively. But, interestingly, x = 0.6 nanocomposite exhibited the negative dielectric behavior having the dielectric constant (ε') ~ -58.5 and dielectric loss (ε") ~ -417 at 8 MHz. Likewise, x = 0.6 sample showed ac-electrical conductivity (σac) -0.159 S/cm at 6 MHz. Hence, these kinds of materials can provide high charge stored capacitor, and perfect absorber applications.