The ferroelectric PZT/odd-odd nylon composite have recently generated interest for high temperature applications. The purposes of this work were to prepare series of PZT/odd-odd nylons composited and study their electrical properties such as relative permittivity and piezoelectric to access their potential for high temperature applications. The commercial PZT powders (PZT850, APC International Ltd.) were used for composite fabrication. The odd-odd nylons used in this study had three distingusished repeating units in the nylons chain. i.e., nylon-57, nylon-77 and nylon-97. The 0-3 composites of PZT/odd-odd nylons with various nylon chains were prepared such as PZT/nylon 57, PZT/nylon 77 and PZT/nylon 97 composites. Composite materials with PZT volume fraction ranging 0.1 to 0.7 were fabricated using the combined techniques of solvent casting and hot pressing to ensure the homogeneous dispersion of PZT powder in the polymer matrix. Experimental results showed that PZT/nylon 57 composites offered the best properties among those composite materials. The electrical properties of composites were strongly dependent on the PZT volume fraction. It was found that the relative permittivity and piezoelectric strain coefficient increased with increasing PZT volume fraction.