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Powerful soft actuators that can perform programmable actuations are highly desired for the development of soft robotics. Herein, we report a moisture-driven polymer actuator, PPA, which is a composite of poly­(3,4-ethylenedioxythiophene)/polyvinyl alcohol/copolymer of acrylic acid and 2-acrylanmido-2-methylpropanesulfonic acid. PPA can not only generate powerful actuation with a contractile stress up to 13 MPa, but can also perform programmable helical motions. PPA films with internal stress along the radial directions were prepared by a simple solution-casting method. Driven by moisture, rectangular strips cut from the same PPA film but with different cutting angles (the oblique angle between the long axis of the PPA strip and the radial axis of the PPA film) can perform direct bending and left-handed or right-handed helical motions, demonstrating the generation of chirality from asymmetric internal stress. By modulating the distribution of internal stress in PPA strips, their moving direction and speed are readily prescribed. The powerful and programmable PPA strips can be used to make soft devices, such as moisture-responsive switches and transporters. Our strategy of generating and utilizing internal stress in responsive polymers represents a promising platform for fabricating smart soft actuators.

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A one‐step synthesis of Li‐rich layered materials with layered/spinel heterostructure has been systematically investigated. The composites are synthesized by a polyol method followed with an annealing process at 500–900 °C for 12 h. A spinel to layer phase transition is considered to take place during the heat treatment, and the samples obtained at different temperatures show diverse phase compositions. An “Li‐rich spinel phase decomposition” phase transition mechanism is proposed to explain the formation of such a heterostructure. The electrochemical properties of the heterostructure are found to be associated with the ratio of spinel to layer phases, the leach out of rock salt phase, and the change of crystallinity and particle size. Product with improved cyclic and rate performance is achieved by annealing at 700 °C for 12 h, with a discharge capacity of 214 mA h g−1 remaining at 0.2 C after 60 cycles and discharge capacity of about 200 mA h g−1 at 1 C.