Bridging In‐Plane Order to Macroscopic Isotropic Ultralight MXene–Graphene Aerogels

Precise nanosheet organization across length scales remains a challenge in translating the intrinsic properties of two‐dimensional (2D) materials into macroscopic porous architectures. Extending in‐plane nanosheet order to long‐range, three‐dimensional (3D) frameworks without structural collapse has been elusive. Here, we report an ultralight MXene–graphene aerogel that exhibits isotropic nanosheet organization spanning from the nanoscale to macroscopic porous networks. This architecture is realized through alginate‐induced liquid‐crystalline assembly coupled with rapid ice‐nucleation‐driven compaction. The isotropic framework homogenizes capillary stresses during drying, enabling ambient‐pressure fabrication of aerogels with an ultralow density of 9.0 mg cm − 3 . Continuous long‐range, in‐plane isotropic stacking of nanosheets enables efficient electron transport along the pore walls, resulting in enhanced electromagnetic interference (EMI) shielding performance. This work establishes a general strategy for constructing porous multiscale isotropic nanosheet architectures.