With the growing popularity of electrical communication equipment, high-performance electromagnetic interference (EMI) shielding materials are widely used to deal with radiation pollution. However, the large thickness and poor mechanical properties of many EMI shielding materials usually limit their applications. In this study, ultrathin and highly flexible TiCT (d-TiCT , MXene)/cellulose nanofiber (CNF) composite paper with a nacre-like lamellar structure is fabricated via a vacuum-filtration-induced self-assembly process. By the interaction between one-dimensional (1D) CNFs and two-dimensional (2D) d-TiCT MXene, the binary strengthening and toughening of the nacre-like d-TiCT /CNF composite paper has been successfully achieved, leading to high tensile strength (up to 135.4 MPa) and fracture strain (up to 16.7%), as well as excellent folding endurance (up to 14 260 times). Moreover, the d-TiCT /CNF composite paper exhibits high electrical conductivity (up to 739.4 S m) and excellent specific EMI shielding efficiency (up to 2647 dB cm g) at an ultrathin thickness (minimum thickness 47 μm). The nacre-inspired strategy in this study offers a promising approach for the design and preparation of the strong integrated and flexible MXene/CNF composite paper, which may be applied in various fields such as flexible wearable devices, weapon equipment, and robot joints.

Robust, stretchable, and strain-sensitive hydrogels have recently attracted immense research interest because of their potential application in wearable strain sensors. The integration of the synergistic characteristics of decent mechanical properties, reliable self-healing capability, and high sensing sensitivity for fabricating conductive, elastic, self-healing, and strain-sensitive hydrogels is still a great challenge. Inspired by the mechanically excellent and self-healing biological soft tissues with hierarchical network structures, herein, functional network hydrogels are fabricated by the interconnection between a "soft" homogeneous polymer network and a "hard" dynamic ferric (Fe) cross-linked cellulose nanocrystals (CNCs-Fe) network. Under stress, the dynamic CNCs-Fe coordination bonds act as sacrificial bonds to efficiently dissipate energy, while the homogeneous polymer network leads to a smooth stress-transfer, which enables the hydrogels to achieve unusual mechanical properties, such as excellent mechanical strength, robust toughness, and stretchability, as well as good self-recovery property. The hydrogels demonstrate autonomously self-healing capability in only 5 min without the need of any stimuli or healing agents, ascribing to the reorganization of CNCs and Fe via ionic coordination. Furthermore, the resulted hydrogels display tunable electromechanical behavior with sensitive, stable, and repeatable variations in resistance upon mechanical deformations. Based on the tunable electromechanical behavior, the hydrogels can act as a wearable strain sensor to monitor finger joint motions, breathing, and even the slight blood pulse. This strategy of building synergistic "soft and hard" structures is successful to integrate the decent mechanical properties, reliable self-healing capability, and high sensing sensitivity together for assembling a high-performance, flexible, and wearable strain sensor.

HIGHLIGHTS • An ultrathin and flexible carbon nanotubes/MXene/cellulose nanofibrils composite paper with gradient and sandwich structure was successfully fabricated via a facile alternating vacuum-assisted filtration process. • The composite paper exhibits excellent mechanical property and electromagnetic interference shielding performance.