Facile Design of Flexible, Strong, and Highly Conductive MXene‐Based Composite Films for Multifunctional Applications

Abstract Strong, conductive, and flexible materials with improving ion accessibility have attracted significant attention in electromagnetic interference (EMI) and foldable wearable electronics. However, it still remains a great challenge to realize high performance at the same time for both properties. Herein, a microscale structural design combined with nanostructures strategy to fabricate TOCNF(F)/Ti 3 C 2 T x (M)@AgNW(A) composite films via a facile vacuum filtration process followed by hot pressing (TOCNF = TEMPO‐oxidized cellulose nanofibrils, NW = nanowires) is described. The comparison reveals that different microscale structures can significantly influence the properties of thin films, especially their electrochemical properties. Impressively, the ultrathin MA/F/MA film with enhanced layer in the middle exhibits an excellent tensile strength of 107.9 MPa, an outstanding electrical conductivity of 8.4 × 10 6 S m −1 , and a high SSE/t of 26 014.52 dB cm 2 g −1 . The assembled asymmetric MA/F/MA//TOCNF@CNT (carbon nanotubes) supercapacitor leads to a significantly high areal energy density of 49.08 µWh cm −2 at a power density of 777.26 µW cm −2 . This study proposes an effective strategy to circumvent the trade‐off between EMI performance and electrochemical properties, providing an inspiration for the fabrication of multifunctional films for a wide variety of applications in aerospace, national defense, precision instruments, and next‐generation electronics.