This study investigates the effect of uniformly coated CNT with ZnO nanoparticles (ZnO@CNT) addition on the dielectric properties of ZnO@CNT/polyvinylidene fluoride (PVDF) hybrid nanocomposites. As a dielectric material, the ZnO@CNT/PVDF nanocomposites were prepared at various loadings of ZnO@CNTs by melt mixing, and they exhibited excellent dielectric properties in X-band frequency (8.2-12.4 GHz). The dielectric study showed that introducing ZnO nanoparticles on the surface of CNT improved dielectric properties by decreasing the dielectric loss tremendously. We attribute the low dielectric loss of the hybrid nanocomposites to the role of ZnO on hindering the CNT direct contact. The mechanism for dielectric properties of these nanocomposites has been explained in detail in the manuscript. This excellent dielectric properties of ZnO@CNT/PVDF would be beneficial for various flexible capacitors, such as embedded capacitors in printed circuit boards.