necessary features has captured enormous scientific attentions.In particular, intrinsically conductive polymers (ICPs) have gained a special status among the promising EMI shielding materials. Among the large family of ICPs, polyaniline (PANI) is one of the prominent polymers, primarily owing to its fascinating properties, such as high electrical conductivity, ease of fabrication, unique controlled chemical and physical properties, as well as low cost. [3] Recently, PANI-based composite has aroused great interest due to the magnified or enhanced electromagnetic properties compared to their bulk counterpart. [4] Various components, such as carbon material, barium titanate (BaTiO 3 ), and bagasse fiber have been adopted to prepare the composites. For example, multi-walled carbon nanotube (MWCNT)/PANI nanocomposites possess a total EMI shielding effectiveness (SE) of ≈39.2 dB at the thickness of 2.0 mm, which is attributed to the synergistic effect of two complementary MWCNT and PANI phases. [5] Due to the optimized dielectric and electrical properties, an excellent SE of 71.5 dB was achieved for BaTiO 3 /PANI nanocomposites with the thickness of 2.7 mm. [6] Compared to pristine PANI, the core-shelled bagasse fiber@PANI composite exhibits immense potential for EMI shield with higher attenuation performance due to the synergistic and interfacial effects. [4b] It is noteworthy that in above cases the structure of PANI is a key parameter that determines its properties and application. Therefore, the delicate regulation and control of highly ordered PANI structures are highly desirable.On the other hand, inspired by natural materials, the designed helical structures endow materials the unique electrical and magnetic performance. Motojima et al. reported the microwave can be significantly attenuated by the helical structure, because of the effective generation of an inductive current. [7] Most recently, Yang et al. reported that PANI with a helical superstructure was produced by co-self-assembly process combined with emulsion droplets methods. The enhanced microwave absorption ability was achieved due to the supramolecular chirality. [8] So, the helical structure is expected to produce excellent EMI shielding performances. But as of yet, sparse research has concentrated on the effect of spiral structure on the shielding properties of PANI-based composites and their underlying mechanism. Furthermore, the EMI shielding capability of the PANI-based helical composite lacks sufficient theoretical Herein, a unique, 3D helical composite with excellent electromagnetic interference (EMI) shielding capability is fabricated. The alkali treated natural cotton fiber (NaCF) is adopted as the helical templet. The compacted polyaniline (PANI) clusters are grafted over NaCF surface via in situ polymerization technology. The correlation between structure and electromagnetic characteristics is investigated in details. The high doping degree and high crystalline phase of PANI coating layer results in the enhanced electrical conductivit...