This study examined the effects of matrix (PVA and Si) on the properties of TEMPO-treated nanocomposites preparing from different pulp sources (Kraft and NaBH4 treated Kraft). Chemical characterization and crystallization were determined via FT-IR, thermal stability via TGA and morphological alterations via SEM. UTM and DTMA were used to measure the Young's and storage moduli. The real and imaginary parts of permittivity and electric modulus were evaluated using an impedance analyzer. After interaction, prominent vibrations and alteration of crystallinity were seen. Storage and Young's moduli decreased after Si and PVA interaction. The Si-TOCN films showed higher permittivity properties and all of the films followed a similar trend of significantly dropping epsilon' and epsilon'' values at high frequency. The PVA-TOCN films had mechanical advantages at room temperature compared to the Si-TOCN films. However, the Si-TOCN films had better thermomechanical properties at high temperatures. NaBH4 revealed favorable effects on mechanical properties of the films.