The piezoelectric performance of polyvinylidene fluoride (PVDF) is shown to double through the controlled incorporation of carbon nanomaterial. Specifically, PVDF composites containing carbon fullerenes (C 60 ) and single-walled carbon nanotubes (SWNT) are fabricated over a range of compositions and optimized for their Young's modulus, dielectric constant, and d 31 piezoelectric coefficient. Thermally stimulated current measurements show a large increase in internal charge and polarization in the composites over pure PVDF. The electromechanical coupling coefficients (k 31 ) at optimal loading levels are found to be 1.84 and 2 times greater than pure PVDF for the PVDF-C 60 and PVDF-SWNT composites, respectively. Such property-enhanced nanocomposites could have significant benefit to electromechanical systems employed for structural sensing, energy scavenging, sonar, and biomedical imaging. V C 2012 American Institute of Physics.