Self-assembled buckypapers have been successfully prepared using sodium carboxyl methyl cellulose (CMC) as a binder. The lowest resistivity that was reached was 0.43 ± 0.03 Ω·m, when the buckypapers were prepared by the same mass of CMC and carboxy-modified carbon nanotubes (CNTs). A heat-resistant electroconductive nanocomposite with epoxy resin as the matrix and CMC/buckypapers as the reinforcement was fabricated by a resin impregnation molding technique. The effects of CMC/buckypaper layers on the conductivity, thermal stability, and mechanical and dynamic mechanical performance of the epoxy resin polymer nanocomposites were investigated. It was found that CMC/buckypapers hold great promise for improving the properties of nanocomposites, and the buckypapers’ performance can be enhanced by using modified CNTs to prepare them. The obtained nanocomposites showed an approximate 71.23% bending strength improvement (125.04 ± 5.62 MPa) and a 30.71% bending modulus improvement (5.83 ± 0.68 GPa), with an increased number of CMC/buckypaper layers. An enhanced degradation temperature and residual mass were also achieved for the nanocomposites when compared with a pure polymer. The nanocomposites with four CMC/buckypaper layers possessed the highest storage modulus (1934 MPa), which was approximately 60% higher than that of a neat polymer (1185 MPa). Therefore, CMC/buckypapers could be effectively used to manufacture heat-resistant electroconductive polymer nanocomposites with improved properties.
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