Ice-Crystal-Templated “Accordion-Like” Cellulose Nanofiber/MXene Composite Aerogels for Sensitive Wearable Pressure Sensors

[Image: see text] Exfoliated MXene nanosheets are integrated with cellulose nanofibers (CNFs) to form composite aerogels with high electric conductivity. The combination of CNFs and MXene nanosheets forms a unique “accordion-like” hierarchical architecture with MXene-CNF pillared layers through ice-crystal templating. Benefiting from the special “layer-strut” structure, the MXene/CNF composite aerogels have low density (50 mg/cm(3)), excellent compressibility and recoverability, as well as superior fatigue resistance (up to 1000 cycles). When being used as a piezoresistive sensor, the composite aerogel exhibits high sensitivity upon different strains, stable sensing performance with various compressive frequencies, broad detection range, and quick responsiveness (0.48 s). Moreover, the piezoresistive sensors are shown to have an excellent real-time sensing ability for human motions such as swallowing, arm bending, walking, and running. The composite aerogels also have a low environmental impact with the natural biodegradability of CNFs. The designed composite aerogels can serve as a promising sensing material for developing next-generation sustainable and wearable electronic devices.