This review focuses on surface modifications of liquid metal (LM). Gallium (Ga) and Ga-based LMs show the promising ability to maintain metallic properties under large mechanical strains when encapsulated inside an elastomer matrix. [1-7] This property is useful in a variety of applications, including wearable/deformable devices, sensors, and soft actuators-the focus of this special issue. There are several motives for creating soft and stretchable devices. For example, devices that are soft and flexible can make conformal contact to human skin for continuous and long-term monitoring. [8-11] Likewise, devices assembled on or within soft robots can maintain function during actuation (bending or stretching) while sensing dynamic motion. Conventional conductors in electronic systems are typically rigid (e.g., copper) and thus poorly suited for soft and stretchable devices. To address this issue, efforts have been taken to create stretchable and deformable conductors using thin metal films with special geometries [12-14] (e.g., pop-up and serpentine electrodes) on a deformable substrate or polymer composites filled with conductive nanomaterials in a stretchable matrix. [15,16] These approaches effectively render rigid materials stretchable through clever engineering of their geometry. However, due to the inherently nonstretchable nature of solid metal films or solid conductive particles, these components/inclusions would add to the overall rigidity of the composite and limit their deformability. LMs are interesting as stretchable conductors because they have metallic conductivity and deformability defined primarily by the encasing material (e.g., elastomer).