Soft, stretchable, and smart strain-sensing hydrogels have attracted significant attention due to their broad applicability in emerging fields. However, developing hydrogel-based strain-sensing materials with finely tuned mechanical and sensing properties remains challenging, primarily due to the inherent brittleness of traditionally fabricated hydrogels. In this study, a novel flexible strain- and epidermis-sensitive sensor was designed using a cellulose nanocrystal (CNC)-mediated acid functionalized multiwalled carbon nanotube (A-MWCNT)-reinforced double-network conductive hydrogel. This dual-network hydrogel system was fabricated by integrating a covalently crosslinked acrylamide (Amm) and [2-(acryloyloxy) ethyl] trimethyl-ammonium chloride (AETAC) with a physically crosslinked network of A-MWCNTs, which were uniformly dispersed via CNCs. Incorporating hydrogen bonding and strong electrostatic interactions within the physical network introduced reversible sacrificial bonds, significantly enhancing the hydrogel's mechanical strength. The hydrogel exhibited mechanical and sensing performance, including sufficient stretchability (431.6%), remarkable sensitivity, a gauge factor (GF) of 4.32 at 400% strain, toughness of 65.6 kJ m⁻³, Young's modulus of 1.5 kPa, and rapid response and recovery times of 100 msec. Furthermore, it demonstrated excellent cycling stability over 100 cycles and effective sensing capabilities across a broad strain range, from small deformations (5%) to large strains (400%). The conductivity of 0.09 S m⁻¹, facilitated by the formation of conduction pathways through the AETAC and A-MWCNTs, further enhanced its performance. Moreover, the hydrogel exhibited practical applicability in detecting various large-scale and physiological human movements. Functioning as a wearable electronic skin, it represents a highly flexible and adaptable material suitable for applications in soft robotics, flexible sensors, and health monitoring devices.

Metal organic frameworks (MOFs) have garnered significant attention in the development of stretchable and wearable conductive hydrogels for flexible transducers. However, MOFs used in hydrogel networks have been hampered by low mechanical performance and poor dispersibility in aqueous solutions, which affect the performance of hydrogels, including low toughness, limited self-recovery, short working ranges, low conductivity, and prolonged response–recovery times. To address these shortcomings, a novel approach was adopted in which micelle co-polymerization was used for the ex situ synthesis of Zn-MOF-based hydrogels with exceptional stretchability, robust toughness, anti-fatigue properties, and commendable conductivity. This breakthrough involved the ex situ integration of Zn-MOFs into hydrophobically cross-linked polymer chains. Here the micelles of EHDDAB had two functions, first they uniformly dispersed the Zn-MOFs and secondly they dynamically cross-linked the polymer chains, profoundly influencing the mechanical characteristics of the hydrogels. The non-covalent synergistic interactions introduced by Zn-MOFs endowed the hydrogels with the capacity for high stretchability, high stress, rapid self-recovery, anti-fatigue properties, and conductivity, all achieved without external stimuli. Furthermore, hydrogels based on Zn-MOFs can serve as durable and highly sensitive flexible transducers, adept at detecting diverse mechanical deformations with swift response–recovery times and high gauge factor values. Consequently, these hydrogels can be tailored to function as wearable strain sensors capable of sensing significant human joint movements, such as wrist bending, and motions involving the wrist, fingers, and elbows. Similarly, they excel at monitoring subtle human motions, such as speech pronunciation, distinguishing between different words, as well as detecting swallowing and larynx vibrations during various activities. Beyond these applications, the hydrogels exhibit proficiency in distinguishing and reproducing various written words with reliability. The Zn-MOF-based hydrogels hold promising potential for development in electronic skin, medical monitoring, soft robotics, and flexible touch panels.