A novel dielectric nanocomposite containing a high permittivity polymer, cyanoethylated cellulose (CRS) and TiO2 nanoparticles was successfully prepared with different weight percentages (10%, 20% and 30%) of TiO2. The intermolecular interactions and morphology within the polymer nanocomposites were analysed. TiO2/CRS nanofilms on SiO2/Si wafers were used to form metal-insulator-metal type capacitors. Capacitances and loss factors in the frequency range of 1 kHz-1 MHz were measured. At 1 kHz CRS-TiO2 nanocomposites exhibited ultra high dielectric constants of 118, 176 and 207 for nanocomposites with 10%, 20% and 30% weight of TiO2 respectively, significantly higher than reported values of pure CRS (21), TiO2 (41) and other dielectric polymer-TiO2 nanocomposite films. Furthermore, all three CRS-TiO2 nanocomposites show a loss factor <0.3 at 1 kHz and low leakage current densities (10(-6)-10(-7) A cm(-2)). Leakage was studied using conductive atomic force microscopy and it was observed that the leakage is associated with TiO2 nanoparticles embedded in the CRS polymer matrix. A new class of ultra high dielectric constant hybrids using nanoscale inorganic dielectrics dispersed in a high permittivity polymer suitable for energy management applications is reported.