Efficient electromagnetic interference (EMI) shielding materials with high flexibility, thin thickness, excellent mechanical property, and superior EMI shielding performance are urgently needed for modern electronic devices in areas of aerospace, military, and wireless communication systems. Herein, highly flexible multi-walled carbon nanotubes (MWCNTs)/aramid fibers (ANFs) composite papers with ordered and layered structures were successfully fabricated via a facile vacuum-assisted filtration. The obtained composite papers exhibited high electrical conductivity, outstanding mechanical property, excellent EMI shielding performance of 41.7 dB at a low density of 0.7–0.8 g cm⁻³ and an average thickness of 0.3 mm. A parameter of the specific shielding effectiveness/thickness (SSE/t) was as high as 2395.8 dB cm² g⁻¹, which was benefited from the layer structures and the formation of conductive networks inside composite papers. It is expected to provide a promising strategy to prepare high-performance nanocomposite papers for EMI shielding in the field of artificial intelligence or smart and wearable electronics.

航空航天、军事和无线通信系统领域的现代电子设备迫切需要具有高柔韧性、薄厚度、优异机械性能和优异EMI屏蔽性能的高效电磁干扰（EMI）屏蔽材料。在此，通过简便的真空辅助过滤成功地制造了具有有序和层状结构的高柔性多壁碳纳米管（MWCNTs）/芳纶纤维（ANFs）复合纸。所获得的复合纸表现出高导电性、优异的机械性能，在0.7-0.8 g cm ^{-3 的}低密度和0.3 mm的平均厚度下具有41.7 dB的优异EMI屏蔽性能。比屏蔽效能/厚度(SSE/t)的一个参数高达2395.8 dB cm²  g ^-1，这得益于复合纸内部的层结构和导电网络的形成。有望为人工智能或智能可穿戴电子领域制备用于EMI屏蔽的高性能纳米复合纸提供一种有前景的策略。