Nanocrystalline CdS impregnated cellulose nanocrystals (CdS-Cellulose) were embedded in polyvinylidene fluoride (PVDF) matrix and free-standing flexible films of CdS-cellulose/PVDF nanocomposite were made by sol-gel technique. Effect of CdS loadings in cellulose embedded in the host matrix (PVDF) on the impedance properties was studied critically for the above samples. Dielectric constants were studied as a function of frequencies (1-100 kHz) at room temperatures. The dielectric constant increased significantly in CdS-cellulose/PVDF nanocomposite than that for pristine PVDF film. The higher values of dielectric constant as well as dielectric loss were obtained at lower frequencies. This may be caused due to contributions arising out of space charge, dipole, and electronic polarizations. At higher frequencies, only dipole and electronic polarization were seen to contribute significantly. The nature of the Cole-Cole plots could be seen to deviate significantly from one impedance semicircular arc before diverging after a frequency of 3,158, 2,147, and 1,925 Hz for CdS-cellulose/PVDF nanocomposite with increased loading of CdS. POLYM. ENG. SCI., 58:1419-1427, 2018. (c) 2017 Society of Plastics Engineers