Polyvinyl alcohol (PVA) composite thin films were prepared using graphene nanoplatelets (GNPs) and multiwalled carbon nanotubes (MWCNTs) as carbon fillers (CFs). The resulting electrical, optical, mechanical, and structural changes caused by adding the CFs to the pure PVA matrix were characterized. The improvement of electrical, optical, and mechanical properties was interpreted in terms of the percolation theory. Depending on this interpretation, the percolation threshold values, and the critical exponential values of the related properties were calculated. It turns out that the measured mechanical and optical changes were compatible with the site percolation theory while the electrical conductivity was compatible with the classical percolation theory. X-ray diffraction (XRD) measurements were performed to correlate the physical properties with the structure of the PVA composite films. They revealed that the degree of crystallinity of the composites increased with the CF reinforcement and that MWCNT was more effective in improvement of the crystallinity of the PVA composites than GNP.
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