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The introduction of three-dimensional (3D) continuous conformations in polymer materials is a convincing proposal for acquiring the desirable multifunction to fulfill the urgent demands of highly integrated electronic devices. However, the limited functional design of the filled aligned network remains challenging. Herein, directional self-assembly 3D MXene/graphene aerogels are fabricated as conductive networks for polyethylene glycol (PEG) matrix. Based on the uniaxial and biaxial ice template method, the temperature gradient affects the aligned arrangement of the 3D microstructure. The biaxial PEG/MXene/GR composites exhibit an enhanced through-plane thermal conductivity of 1.64 W m −1 K −1 at 10.6 vol % content, which is 522% higher than that of pure PEG. The influence of the biaxial self-assembly strategy compared with that of the uniaxial one on the thermal conductivity reaches the highest 333% when the weight ratio equals 1:1. Meanwhile, the same difference also occurs in the electromagnetic shielding interference (EMI) property. The advanced EMI-shielding effectiveness of the biaxial PM1G1 composites reaches ∼36 dB at the 2.5 mm thickness. This research provides valuable guidance for designing highperformance applications of anisotropic thermal management and EMI shielding in 5G telecommunications and mobile electronic devices.

The multi-functionalization of polymer composites refers to the ability to connect multiple properties through simple structural design and simultaneously achieve multi-performance optimization. The large-scale design and mass production to realize the reasonable structure design of multifunctional polymer composites are urgently remaining challenges. Herein, the multifunctional MXene/graphene/polymer composites with three-dimensional thermally and electrically conductive network structures are fabricated via the utilization of the microstructure of the soft template, and a facile dispersion dip-coating approach. As a result, the polymer composites have a multi-performance improvement. At the MXene and graphene content of 18.7 wt%, the superior through-plane thermal conductivity of polymer composite is 2.44 W m−1 K−1, which is 1118% higher than that of the polymer matrix. The electromagnetic interference (EMI) shielding effectiveness of the sample reaches 43.3 dB in the range of X-band. And the mechanical property of the sample has advanced 4 times compared with the polymer matrix. The excellent EMI shielding and thermal management performance, along with the effortless and easy-to-scalable producing techniques, imply promising perspectives of the polymer composites in the next-generation smart electronic devices.

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