Multi‐Field Synergy for Orchestrating Filler Angles in Polyimide Aerogels with Switchable Electromagnetic Interference Shielding

The fast-evolving IT sector necessitates intelligent electromagnetic interference (EMI) shielding materials capable of real-time, environment-responsive. While current approaches based on reconstructing conductive networks through mechanical strain enable dynamically responsive shielding, but face a narrow tuning range, inadequate stability, and practical limitations. To address this, we propose an electric/magnetic field synergistic regulation strategy. This approach enables precise control over the alignment angle between reduced graphene oxide (rGO) and nickel nanowires (NiNWs) by manipulating the external field direction, producing rGO@NiNWs/polyimide aerogels with 3D ordered networks. Leveraging this design, the aerogels achieve reversible, wide-range tuning of EMI shielding performance through simple physical rotation, enabling reliable "on/off" switching capability. The oriented structure also optimizes both filler interconnection efficiency and interfacial polarization. With an rGO@NiNWs content of 80 wt.% and an inter-phase angle of 90°, the aerogels demonstrate excellent ultra-wideband EMI shielding performance across gigahertz and terahertz bands, with an average shielding effectiveness of 85 dB in the terahertz band, alongside good stability in extreme environments. Finite element simulations further reveal how the spatial configuration of rGO@NiNWs governs the shielding behavior and intelligent response mechanism. This study paves the way for next-generation intelligent electromagnetic protection materials, with promising potential for aerospace and wearable applications.