Hydrogels, as classic soft materials, are important materials for tissue engineering and biosensing with unique properties, such as good biocompatibility, high stretchability, strong adhesion, excellent self-healing, and self-recovery. Conductive hydrogels possess the additional property of conductivity, which endows them with advanced applications in actuating devices, biomedicine, and sensing. In this review, we provide an overview of the recent development of conductive hydrogels in the field of strain sensors, with particular focus on the types of conductive fillers, including ionic conductors, conducting nanomaterials, and conductive polymers. The synthetic methods of such conductive hydrogel materials and their physical and chemical properties are highlighted. At last, challenges and future perspectives of conductive hydrogels applied in flexible strain sensors are discussed.

Recently, flexible sensors based on conductive hydrogels have been widely used in human health monitoring, human movement detection and soft robotics due to their excellent flexibility, high water content, good biocompatibility. However, traditional conductive hydrogels tend to freeze and lose their flexibility at low temperature, which greatly limits their application in a low temperature environment. Herein, according to the mechanism that multi−hydrogen bonds can inhibit ice crystal formation by forming hydrogen bonds with water molecules, we used butanediol (BD) and N−hydroxyethyl acrylamide (HEAA) monomer with a multi−hydrogen bond structure to construct LiCl/p(HEAA−co−BD) conductive hydrogel with antifreeze property. The results indicated that the prepared LiCl/p(HEAA−co−BD) conductive hydrogel showed excellent antifreeze property with a low freeze point of −85.6 °C. Therefore, even at −40 °C, the hydrogel can still stretch up to 400% with a tensile stress of ~450 KPa. Moreover, the hydrogel exhibited repeatable adhesion property (~30 KPa), which was attributed to the existence of multiple hydrogen bonds. Furthermore, a simple flexible sensor was fabricated by using LiCl/p(HEAA−co−BD) conductive hydrogel to detect compression and stretching responses. The sensor had excellent sensitivity and could monitor human body movement.

Bilayer hydrogel actuators, consisting of an actuating layer and a functional layer, show broad applications in areas such as soft robotics, artificial muscles, drug delivery and tissue engineering due to their inherent flexibility and responses to stimuli. However, to achieve the compatibility of good stimulus responses and high mechanical properties of bilayer hydrogel actuators is still a challenge. Herein, based on the double-network strategy and using the synchronous ultraviolet (UV) polymerization method, an upper critical solution temperature (UCST)-type bilayer hydrogel actuator was prepared, which consisted of a poly(acrylamide-co-acrylic acid)[MC] actuating layer and an agar/poly(N-hydroxyethyl acrylamide-co-methacrylic acid)[AHA] functional layer. The results showed that the tensile stress/strain of the bilayer hydrogel actuator was 1161.21 KPa/222.07%. In addition, the UCST of bilayer hydrogels was ~35 °C, allowing the bilayer hydrogel actuator to be curled into an “◎” shape, which could be unfolded when the temperature was 65 °C, but not at a temperature of 5 °C. Furthermore, hydrogel actuators of three different shapes were designed, namely “butterfly”, “cross” and “circle”, all of which demonstrated good actuating performances, showing the programmable potential of bilayer hydrogels. Overall, the bilayer hydrogels prepared using double-network and synchronous UV polymerization strategies realized the combination of high mechanical properties with an efficient temperature actuation, which provides a new method for the development of bilayer hydrogel actuators.