Flexible piezoelectric nanocomposites have been the subject of a lot of recent research due to the development and use of wearable electronic devices and the increasing need for new harvesting devices and sensors due to increasingly intelligent and interconnected cities. In this study, flexible piezoelectric nanocomposites using elastomeric polyurethane (PU) as matrix, and lead zirconate titanate (PZT) as active phase, were produced using cellulose nanocrystals (CNC) as the third phase. The study describes the effect of CNC insertion on the morphology, thermal, electrical, and piezoelectric properties of the nanocomposites. It points out that the CNCs not only act to cause greater dispersion of the ceramic grains in the matrix, but also to lead to greater polarization effectiveness of the ceramic grains, resulting in a longitudinal piezoelectric coefficient (d33) increase of more than 370%, as compared with biphasic composites dependent on the ceramic and nanocrystals content.