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• 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]