AbstractSoft actuators can harvest environmental energy and convert it into kinetic energy for motions like bending, twisting, stretching, and contracting. However, it remains challenging to design soft film actuators for complex and programmable deformation in three dimensions. Herein, a weldable and patternable multi‐stimuli‐responsive bilayer soft actuator is developed by a mask‐assisted spraying coating process, and its 3D geometries are achieved by welding the sodium alginate (SA) layer using water. The intrinsic hygroscopicity of SA film and the magnetic and photothermal properties of Fe3O4 nanoparticles enable reversible deformation of the bilayer actuator under three different external stimuli: moisture, magnetic field, and sunlight. Based on these properties, a variety of multi‐stimuli‐responsive intelligent devices are developed including smart curtains, smart grippers, biomimetic walkers, rolling actuators, swimmers, and windmill rotators. All these actuating stimulations are derived from naturally renewable energy without the consumption of any artificial energy, providing important enlightenment for green and sustainable applications of soft actuators.
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