Entangled hydrogels: physicochemical properties, synthesis and applications

Abstract Recent advancements in soft robotics have catalyzed significant progress in smart materials research, positioning hydrogel-based actuators as promising candidates for bioinspired soft robotic systems owing to their tunable mechanical properties and inherent flexibility. A central challenge lies in balancing the retention of desirable mechanical properties with achieving high responsiveness in hydrogel-based soft robotic devices. Entangled polymer networks have emerged as a groundbreaking class of materials for soft actuators, offering distinctive mechanical behavior and precisely adjustable responsiveness. This review aims to establish design principles for engineering soft actuators with tailored functionalities by elucidating the underlying mechanisms governing controlled chain entanglement dynamics during material processing. Furthermore, current technical limitations and future research directions are examined from a materials science perspective. This review provides guidance for the design and fabrication of soft actuators with desired properties through a rational route involving controlled chain entanglement.