This study reports on the effects of organic polyvinyl alcohol (PVA) and inorganic silica polymer on properties of Celluclast-treated nanofibrillated cellulose composites. Nanofibrillated cellulose was isolated from Eucalyptus camaldulensis and prior to high-pressure homogenizing was pretreated with Celluclast enzyme in order to lower energy consumption. Three nanocomposite films were fabricated via the casting process: nanofibrillated cellulose (CNF), nanocellulose-PVA (CNF-P)and,nanocellulose-silica (CNF-Si). Chemical characterization, crystallization and thermal stability were determined using FT-IR and TGA. Morphological alterations were monitored with SEM. The Young's and storage moduli of the nanocomposites were determined via a universal testing machine and DTMA. The real and imaginary parts of permittivity and electric modulus were evaluated using an impedance analyzer. The crystallinity values of the nanocomposites calculated from the FT-IR were in agreement with the TGA results, showing that the lowest crystallinity value was in the CNF-Si. The CNF-P displayed the highest tensile strength. At a high temperature interval, the storage modulus of the CNF-Si was greater than that of the CNF or CNF-P. The CNF-Si also exhibited a completed singular relaxation process, while the CNF and the CNF-P processes were uncompleted. Consequently, in terms of industrial applications, although the CNF-P composite had mechanical advantages, the CNF-Si composite displayed the best thermo-mechanical properties. (C) 2017 Elsevier B.V. All rights reserved.