Highly‐Aligned All‐Fiber Actuator with Asymmetric Photothermal‐Humidity Response and Autonomous Perceptivity

Abstract Soft robots adapt to complex environments for autonomous locomotion, manipulation, and perception are attractive for robot‐environment interactions. Strategies to reconcile environment‐triggered actuation and self‐powered sensing responses to different stimuli remain challenging. By tuning the in situ vapor phase solvent exchange effect in continuous electrospinning, an asymmetric highly‐aligned all‐fiber membrane (HAFM) with a hierarchical “grape‐like” nanosphere‐assembled microfiber structure (specific surface area of 13.6 m² g⁻¹) and excellent mechanical toughness (tensile stress of 5.5 MPa, and fracture toughness of 798 KJ m⁻³) is developed, which shows efficient asymmetric actuation to both photothermal and humidity stimuli. The HAFM consists of a metal‐organic framework (MOF)‐enhanced moisture‐responsive layer and an MXene‐improved photothermal‐responsive layer, which achieves substantial actuation with a bending curvature up to ≈7.23 cm⁻¹ and a fast response of 0.60 cm⁻¹ s⁻¹. By tailoring the fiber alignment and bi‐layer thickness ratio, different types of micromanipulators, automatic walking robots, and plant robots with programmable structures are demonstrated, which are realized for self‐powered information perception of material type, object moisture, and temperature by integrating the autonomous triboelectric effect induced by photothermal‐moisture actuation. This work presents fiber materials with programable hierarchical asymmetries and inspires a common strategy for self‐powered organism‐interface robots to interact with complex environments.