Piezoelectric lead zirconate titanate (PZT) ceramic fiber/polymer composites were fabricated by a novel technique referred to as “relic” processing. Basically, this involved impregnating a woven carbon‐fiber template material with PZT precursor by soaking the template in a PZT stock solution. Careful heat treatment pyrolized the carbon, resulting in a PZT ceramic relic that retained the fibrous template form. After sintering, the densified relic was backfilled with polymer to form a composite. Optimized relic processing consisted of soaking activated carbon‐fiber fabric twice in an intermediate concentration (405‐mg PZT/(1‐g solution)) alkoxide PZT solution and sintering at 1285°C for 2 h. A series of piezoelectric composites encompassing a wide range of dielectric and piezoelectric properties was prepared by varying the PZT‐fiber orientation and polymer‐matrix material. In PZT/Eccogel polymer composites with PZT fibers orientated parallel to the electrodes,K= 75,d33= 145 pC/N,dh= 45 ± 5 pC/N, anddhgh= 3150 × 10−15m2/N were measured. Furthermore, in composites with a number of PZT fibers arranged perpendicular to the electroded surfaces,K= 190,d33= 250 pC/N,dh= 65 ± 2 pC/N, andd