This review focuses on surface modifications to gallium‐based liquid metals (LMs), which are stretchable conductors with metallic conductivity and nearly unlimited extensibility due to their liquid nature. Despite the enormous surface tension of LM, it can be patterned into nonspherical shapes, such as wires, due to the presence of a native oxide shell. Incorporating inherently soft LM into elastomeric devices offers comfort, mechanical compliance, and stretchability. The thin oxide layer also enables the formation of stable liquid colloids and LM micro/nanosized droplets that do not coalesce easily. The oxide layer can also be exfoliated and chemically modified into semiconductor 2D materials to create and deposit atomically thin materials at room temperature. Thus, the interface and its manipulation are important. This review summarizes physical and chemical methods of modifying the surface of LM to tune its properties. The surface modification of LM provides unique applications, including use in soft biomedical sensors and actuators with mechanical properties similar to human tissue.