There is ever-increasing interest yet grand challenge in developing programmable untethered soft robotics. Here we address this challenge by applying the asymmetric elastoplasticity of stacked graphene assembly (SGA) under tension and compression. We transfer the SGA onto a polyethylene (PE) film, the resulting SGA/PE bilayer exhibits swift morphing behavior in response to the variation of the surrounding temperature. With the applications of patterned SGA and/or localized tempering pretreatment, the initial configurations of such thermal-induced morphing systems can also be programmed as needed, resulting in diverse actuation systems with sophisticated three-dimensional structures. More importantly, unlike the normal bilayer actuators, our SGA/PE bilayer, after a constrained tempering process, will spontaneously curl into a roll, which can achieve rolling locomotion under infrared lighting, yielding an untethered light-driven motor. The asymmetric elastoplasticity of SGA endows the SGA-based bi-materials with great application promise in developing untethered soft robotics with high configurational programmability.

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