Emulsion‐Based Multiscale Structural Design Realizes Lightweight and Superelastic Graphene Aerogels for Electromagnetic Interference Shielding

Ultralight graphene aerogels with high electrical conductivity and superelasticity are demanded yet difficult to produce. A versatile emulsion‐based approach is demonstrate to optimize multiscale structure of lightweight, elastic, and conductive graphene aerogels. By constructing Pickering emulsion using graphene oxide (GO), poly (amic acid) (PAA), and octadeyl amine (ODA), micron‐level close‐pore structure is realized while thermal shrinkage mismatch between GO and PAA creates numerous nanowrinkles during thermal annealing. GO nanosheets are bridged by PAA‐derived carbon, enhancing the structural integrity at molecular level. These multiscale structural features facilitate rapid electron transport and efficient load transfer, conferring graphene aerogels with intriguing mechanical and electromagnetic interference (EMI) shielding properties. The emulsion‐based graphene aerogel with an ultralow density of ≈3.0 mg cm−3 integrates outstanding electrical conductivity, air‐caliber thermal insulation, high EMI shielding effectiveness of 75.0 dB, and 90% strain compressibility with superb fatigue resistance. Intriguingly, thanks to the gel‐like rheological behavior of the emulsion, ultralight graphene scaffolds with programmable geometries are obtained by 3D printing. This work provides a general approach for the preparation of ultralight and superelastic graphene aerogels with excellent EMI shielding properties, showing broad application prospects in various fields. Superelastic graphene aerogels with multiscale structural tunability are fabricated by an emulsion‐based approach, followed by freeze‐drying and thermal annealing. The aerogels with ultralow density (3.0 mg cm−3) can withstand 90% of reversible compressive strain and exhibit air‐caliber thermal insulation and high electromagnetic interference shielding effectiveness of 75.0 dB in X‐band.