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Inspired by creatures, abundant stimulus-responsive hydrogel actuators with diverse functionalities have been manufactured for applications in soft robotics. However, constructing a shape memory and self-sensing bilayer hydrogel actuator with high mechanical strength and strong interfacial bonding still remains a challenge. Herein, a novel bilayer hydrogel with a stimulus-responsive TEMPO-oxidized cellulose nanofibers/poly(N-isopropylacrylamide) (TOCN/PNIPAM) layer and a non-responsive TOCN/polyacrylamide (TOCN/PAM) layer is proposed as a thermosensitive actuator. TOCNs as a nano-reinforced phase provide a high mechanical strength and endow the hydrogel actuator with a strong interfacial bonding. Due to the incorporation of TOCNs, the TOCN/PNIPAM hydrogel exhibits a high compressive strength (~89.2 kPa), elongation at break (~170.7 %) and tensile strength (~24.0 kPa). The prepared PNIPAM/TOCN/PAM hydrogel actuator performs the roles of an encapsulation, jack, temperature-controlled fluid valve and temperature-control manipulator. The incorporation of Fe3+ further endows the bilayer hydrogel actuator with a synergistic performance of shape memory and temperature-driven, which can be used as a temperature-responsive switch to detect ambient temperature. The PNIPAM/TOCN/PAM-Fe3+ conductive hydrogel can be assembled into a flexible sensor and generate sensing signals when driven by temperature changes to achieve real-time feedback. This research may lead to new insights into the design and manufacturing of intelligent flexible soft robots. [Display omitted] [ABSTRACT FROM AUTHOR]

• A green and common method was proposed to prepare biomimetic actuators. • The PNPB actuator showed excellent multi-stimulus response and synergistic effect. • Anisotropic natural bamboo endowed the PNPB actuator programmable performance. • The PNPB actuator had application potential in complex environment. Hydrogel actuators with controllable deformation and excellent biocompatibility are widely used in soft robot, valve, drug delivery and lenses. However, the stimulation response performance of existing hydrogel actuators mostly focuses on a single active layer, which greatly affects its driving performance and service life. In this work, we integrate temperature-responsive hydrogel (Poly (N-isopropyl acrylamide), PNIPAM) and pH-responsive hydrogel (polyacrylic acid, PAAc) into one system to fabricate a dual active layer composite hydrogel actuator with high performance. Based on the PAAc hydrogels achieving contract or expand at different pH values, the obtained actuator exhibits admirable bidirectional bending characteristics. In addition, the anisotropic bamboo sheet endows the hydrogel actuator with programmable 3 D complex deformation. Benefitting from the synergy and different responsiveness between the two active layers, the hydrogel actuator not only has multiple response performance, but also greatly improves its deformation degree and response speed. More importantly, these promising properties of the actuator have broad application prospects in the development of pattern design and intelligent switch. This work proposes a promising strategy for the structural design of hydrogel actuators with excellent performance, and encourages more exploration of the application range of the actuator. [ABSTRACT FROM AUTHOR]