Leveraging the unique attributes of functional soft materials to generate force and deformation, significant advancements in soft actuators are driving the evolution of smart robotics. Liquid metals (LMs), known for their high deformability and tunable morphology, demonstrate remarkable actuating capabilities through controllable surface tension. Inspired by the predation method of chameleons, this work introduces a bioinspired LM actuator (BLMA) by modulating the morphology of LM. This BLMA enables high‐strain (up to 170%) actuation by precisely directing LM droplets toward an electrode. Various parameters affecting the BLMA's actuating performance are explored. Notably, the application of a reductive voltage induces rapid solidification of supercooled LM, facilitating phase transition at room temperature. The solidified LM enhances its holding force of BLMA by over 1000 times. To underscore the superior capabilities of the BLMA, diverse applications, such as a complex two‐dimensional plane actuator, a stepper motor with adjustable step intervals, a phase transition‐controlled relay, and a laser code lock actuation gate set, are presented. It is anticipated that the exceptional characteristics of the BLMA will propel advancements in the realms of soft robotics and mechatronics.
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