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•Bilayer hydrogels undergo transparent-opaque transitions and shape alterations.•Bilayer hydrogels exhibit adjustable EMI shielding capability.•Poly(N-isopropyl acrylamide) microgel can reduce response time of bilayer hydrogels.•Maximum EMI shielding effectiveness of bilayer hydrogels reaches 27.64 dB.
Thermochromic smart windows with adjustable electromagnetic interference (EMI) shielding capability are integral elements in modernized buildings, especially in military applications, due to their energy-saving benefits and ability to mitigate electromagnetic pollution. However, its application is limited by the relatively poor light transmission of conductive substances and the high demand for light transmission of thermochromic smart windows. Maintaining the thermochromic performance of smart windows while adjusting EMI shielding effectiveness (SE) poses a significant challenge. Here, we propose a straightforward approach to create a smart EMI shielding material with adaptable properties, including light transmission, shape, and EMI SE. This method involves a layer-by-layer polymerisation process followed by solvent substitution. The resulting hydrogel exhibits tunable optical properties, making it suitable for use as a smart window that responds to external conditions and offers local tunability. Noteworthy characteristics include high light transmittance (80.87 %), ultra-fast response time (16 s), multiple shape adjustments, adjustable EMI SE ranging from 0 to 27.64 dB, and strong adhesion, among other features. These findings suggest that the obtained hydrogels have significant potential to provide a substantial advantage in developing next-generation soft and intelligent smart EMI shielding windows.