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• 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]

• The morph-genetic method was innovatively used to fabricate the ABH actuator. • The ABH actuator exhibits promising comprehensive performance. • The assembled biomimetic actuators show excellent synergistic performance. • The biomimetic actuator shows potential for a variety of applications. Stimuli-responsive hydrogels are most promising for the fabrication of autonomous bio-mimetic soft actuators. However, their weak actuation forces and isotropic volume change hinder their practical utilization as versatile actuators, owing to their fragility. Herein, we used the morph-genetic method to fabricate anisotropic bamboo/poly(N-isopropylacrylamide) hydrogel (ABH) complex for use as soft actuator. First of all, the bamboo fiber structure provides an anisotropic framework for the ABH actuator to achieve precise deformational programmability. Secondly, benefiting from the ultra-high directional strength (110 MPa) of bamboo, ABH actuator exhibits sufficiently robust mechanical property, which generates a powerful actuating force. Lastly, owing to the regulation of bamboo sheet and PNIPAM hydrogel, the ABH actuator not only achieves ultra-fast response speed (825°/s of the bending speed), but also has excellent synergetic performance. We demonstrate several bio-mimetic actuating devices based on ABH actuator, inspired by the intricate motions of natural organisms, to highlight how the specific materials properties and their synergy can be systematically exploited for the rational design of soft actuators. Henceforth, it is anticipated that the development of hydrogel actuators could continue to benefit from the use of various naturally-anisotropic materials, such as shape-memory polymers or liquid crystals, for the preparation of further advanced hydrogel actuators by the morph-genetic method. [ABSTRACT FROM AUTHOR]

• PPy-coated P(NIPAM-ABP) electrospun nanofiber can provide high strength. • PPy-coating by in situ polymerization can provide high light-responsive. • The actuator owns ultrafast deformation and rapid recovery. • The actuator can realize various 3D programmable complex deformations. • We have explored new biomimetic devices based on the advantages of the actuator. Intelligent hydrogels are promising for biomimetic actuators, but acquiring actuations with both high speed and powerful force is still extremely difficult. Herein, a new robust polypyrrole (PPy)-coated copoly(isopropylacrylamide-4-benzoylphenyl acrylate) [P(NIPAM-ABP)] electrospun light-responsive hydrogel is explored. The (PPy)-coated P(NIPAM-ABP) hydrogel can be obtained via in-situ polymerization of pyrroles on the nanofiber-oriented electrospun P(NIPAM-ABP) hydrogel. Compared with original P(NIPAM-ABP) hydrogel, this PPy-coated P(NIPAM-ABP) hydrogel can integrate highly-enhanced mechanical strength (from 1.21 to 5.12 MPa of tensile strength) and ultrahigh-efficiency of photothermal conversion together. In addition, the orientation of P(NIPAM-ABP) nanofibers can still maintain well for programmable complex deformations. Consequently, the as-prepared robust bi-hydrogel actuator with ultrafast and complex deformations has been achieved, through bonding the PPy-P(NIPAM-ABP) hydrogel membrane with a polyethylene glycol diacrylate-cellulose nanofiber (PEGDA-CNF) composite hydrogel membrane via interfacial ultraviolet (UV) polymerization of PEGDA monomers. Several light-responsive biomimetic actuating devices have been achieved, which owning powerful force (can grab up 100 times of self-weight), rapid speed (1285.71°/s of folding) or precisely programmable complex deformations. Furthermore, two biomimetic devices with synergistic functions of the three advantages above have been explored, which can mimic the child's sit-up and the starfish's continuous crawling movement respectively. This work provides a robust remotely-controlled light-responsive hydrogel actuator with powerful force, ultrafast speed and programmable complex actuations, which will inspire the design and fabrication of novel soft biomimetic actuating materials and systems. [ABSTRACT FROM AUTHOR]

Near-infrared light-responsive hydrogel actuator with complex deformations and remote precise control is fabricated from the natural bamboo. The resulting biomimetic bamboo/PNIPAM hydrogel actuator can be precisely designed to perform a variety of simulations. [Display omitted] • Biomimetic actuators based on anisotropic natural bamboo were prepared. • Nigrosine was first used to fabricate light-responsive hydrogel actuator. • The actuator exhibits outstanding programmability and remote-control performance. • The actuator can move freely on the water surface based on Marangoni effect. Near-infrared light-responsive hydrogels are one of the most important soft biomimetic actuators owing to their accuracy, remote control performance, and permeability. However, the complex deformations and materials of hydrogel actuators are still a serious challenge. Herein, we have developed a novel composite hydrogel actuator by combining natural bamboo sheet and nigrosine/poly(N-isopropylacrylamide) (PNIPAM) composite hydrogel. The high-efficient photothermal conversion of the nigrosine/PNIPAM composite hydrogel sheet generates light-responsive actuation that is remotely controllable. Furthermore, the bamboo sheet with fiber-oriented structure can be cut at different angles, which facilitates programmable 3D complex deformations in the actuator. Accordingly, we have designed a series of biomimetic actuating devices, including simulations of butterfly antenna, Dendrobium , smart switch, and even a multi-step deformational biomimetic claw. In addition, we also explored a biomimetic insect with precisely-controlled fast movements on the water surface based on Marangoni effect. This work provides a simple but general strategy for fabricating biomimetic actuators and will inspire new designs for intelligent soft actuators. [ABSTRACT FROM AUTHOR]

[Display omitted] • The actuator can achieve synergistic movement of deformation and transportation. • Added Fe 3 O 4 NPs provide both magnetism and high-efficient photothermal conversion. • The hydrogel actuator owns high tensile-strength of 4.59 MPa via electrospinning. • The actuator can provide ultrafast deformational speed of 178°/s. • We have explored new bio-inspired systems with two/multi-step synergic actuation. As a soft/wet intelligent material, hydrogel actuators with multiple stimuli-responsiveness have been widely developed. However, it is still greatly difficult for them to integrate bi/multiple responsiveness together for bio-mimetic synergistic actuation. Here, we have explored a high-strength anisotropic bi-layer hydrogel actuator with P(NIPAM-ABP) layer and Fe 3 O 4 /PAN layer via electrospinning technique, which can provide programmable bi-functional synergistic movement. The Fe 3 O 4 /PAN layer can provide magnetic responsive navigation for long-range transportation on account of the magnetism of the Fe 3 O 4 nanoparticles. Furthermore, the ultrahigh photothermal conversion efficiency of the Fe 3 O 4 nanoparticles in the Fe 3 O 4 /PAN layer, can endow the P(NIPAM-ABP) layer with fast remotely-controlled photothermal-responsive deformation. Most importantly, this hydrogel actuator can achieve complex higher-level programmable movements than before based on the synergy of remotely-controlled deformation and the long-range transportation, which can be utilized to design various novel bio-mimetic soft-robots. Last but not least, the introduction of the electrospinning, not only can achieve high strength (4.59 MPa of tensile strength) of this bi-layer hydrogel, but also can provide both ultrafast (178°/s) and programmable complex photothermal-responsiveness, owing to the ultrahigh specific surface area (ultra-thin and porous structure) and excellent orientation of the thermal-responsive P(NIPAM-ABP) nanofibers respectively. This work will provide a general method via electrospinning for anisotropic hydrogel actuator with bi/multiple-functional synergy and will provide a new strategy for smart actuators and other bio-mimetic intelligent materials/systems. [ABSTRACT FROM AUTHOR]