Nature‐Inspired Functional Aerogel Fibers with Engineerable Core–Shell Morphology

Abstract Aerogels offer exceptional multifunctionality but are often hampered by mechanical fragility, structural brittleness, and complex processing. Inspired by the core–shell architecture of the Canadian goose feather rachis, a scalable coaxial wet‐spinning approach is reported to produce wearable aerogel fibers. Polyimide (PI) shells encapsulating conductive Ti 3 C 2 T x MXene cores are fabricated via a tailored polyamic acid (PAA) solvent/non‐solvent exchange phase‐inversion process. Detailed mechanistic studies show that the ethanol–water ratio in the coagulation bath critically governs phase‐inversion kinetics, structural integrity, and hierarchical porosity. Under optimized conditions, the resulting aerogel fibers exhibit absorption‐dominant EMI shielding (54.9 dB), high mechanical robustness (tensile strength up to 20.4 MPa), and record‐level thermal insulation (thermal conductivity of 21.7 ± 1.5 mW m −1 K −1 ). This innovative chemical strategy provides a practical and scalable route to lightweight, durable, and multifunctional aerogel fibers for wearable electronics, thermal management, and EMI shielding applications.