Nature will always be an endless source of bioinspiration for man‐made smart materials and multifunctional devices. Impressively, even cutoff leaves from resurrection plants can autonomously and reproducibly change their shape upon humidity changes, which goes along with total recovery of their mechanical properties after being completely dried. In this work, simple bilayers are presented as autonomously moving, humidity‐triggered bending actuators. The bilayers—showing reproducible bending behavior with reversible kinematics and multiway behavior—are studied in terms of their mechanical behavior upon humidity changes. The active layer consists of a highly conducting polymer film based on poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) with poly(dimethylsiloxane) (PDMS) as passive layer. The response to humidity is explored with dynamic mechanical thermal analysis and quartz crystal microbalance measurements. Introduction of a composite beam model allows to predict the curvature of the actuators with input from the rheological measurements. It is clearly demonstrated that volumetric strain and Young's modulus, both heavily influenced by the water uptake, dominate the bending behavior and therefore the curvature of the actuators. This loop of rheological characterization coupled with an analytical model allows to predict curvatures of in principle any complex geometry and material combination for moving parts in soft robotics.

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The work demonstrates a novel route to synthesize disorder rich rock salt-type Li2MnO3−δ electrodes flaunting remarkably high capacity due to dynamic phase transformation during cycling.