Composites of polyvinyledene fluoride (PVDF) and strontium barium niobate (SrxBa1−xNb2O6 for x = 0.53/SBN)/ФSBN − (1 − Ф)PVDF with Ф = 0.1 to 0.3 have been prepared by hot uniaxial press. Structural, morphological, dielectric and pyrolectric properties of the composites have been studied. Self-sustaining thick films with a 0–3 connectivity have been synthesized. The dielectric constant (εr) was found to increase with the increase in ceramic volume fraction (Ф) in the composite. The composite with Ф = 0.3 is found to have highest values of pyroelectric coefficient (pi) ~13.475 μC/m2K, FOMI ~0.481 μC/m2K and FOMII ~20.13 μC/m2K with good mechanical flexibility.