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Pristine carbon nanotubes (CNTs) and functionalized carbon nanotubes (f-CNTs) were introduced into conductive poly(methyl methacrylate)/graphene nanoplatelet (PMMA/GNP) composites to achieve a synergistic effect in the enhancement of the conductivity and the reduction in the percolation threshold by forming a 3-Dimensional(3-D) hybrid structure. Both the in-plane and perpendicular electrical properties were investigated. The synergies of hybrid fillers in the in-plane direction were more dependent on the total filler loading, while those in the perpendicular direction were significantly influenced by the GNP/CNT or GNP/f-CNT ratios. Typically, a schematic diagram of the evolution of the 3-D conductive pathways of PMMA/GNP/f-CNT composite at different GNP/f-CNT ratios was presented to explain this phenomenon. Moreover, tunable conductivity anisotropy (defined as the ratio of in-plane conductivity to perpendicular conductivity) ranging from 0.01 to 1000 was achieved, simply by constructing different conductive structures at various filler loadings or ratios in composites. Graphical abstract The synergistic effect of GNPs and f-CNTs varies with the microstructural conductive network evolution at different filler ratios.

Front Cover: A novel theoretical approach is presented to calculate the resistivity below the percolation threshold for carbon‐fiber‐polymer composites yielding an equation for resistivity as a function of degree of filling is determined only by the fiber orientation. An exponent is predicted for the isotropic case and infinite long fibers. This is reported by Guanda Yang, Dirk W. Schubert, Muchao Qu, and Fritjof Nilsson in article number https://doi.org/10.1002/mats.201700105.

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Revealed logarithm longitude electrical conductivity σ∥ and transverse electrical conductivity σ⊥ of PMMA/CF composite filaments.