AbstractLiquid metals, with their unique combination of electrical and mechanical properties, offer great opportunities for actuation based on surface tension modulation. Thanks to the scaling laws of surface tension, which can be electrochemically controlled at low voltages, liquid metal actuators stand out from other soft actuators for their remarkable characteristics such as high contractile strain rates and higher work densities at smaller length scales. This review summarizes the principles of liquid metal actuators and discusses their performance as well as theoretical pathways toward higher performances. The objective is to provide a comparative analysis of the ongoing development of liquid metal actuators. The design principles of the liquid metal actuators are analyzed, including low‐level elemental principles (kinematics and electrochemistry), mid‐level structural principles (reversibility, integrity, and scalability), and high‐level functionalities. A wide range of practical use cases of liquid metal actuators from robotic locomotion and object manipulation to logic and computation is reviewed. From an energy perspective, strategies are compared for coupling the liquid metal actuators with an energy source toward fully untethered robots. The review concludes by offering a roadmap of future research directions of liquid metal actuators.