AbstractAlterable surface tension and electrical properties of liquid metals are of great significance to their applications in intelligent robots, bionic applications, and electronics. To further understand the interfacial properties of liquid metals, the highly effective and in situ modulation strategy is imperative to be developed. Here, a bubble‐induced in situ modulation strategy to achieve the on‐demand surface tension and electrical properties is initially demonstrated. The size and shape of bubbles are modulated by virtue of thermal effect under the laser irradiation. As a consequence of the regulated location of bubbles, the surface tension and electrical potential are in situ adjusted reversibly and periodically. In situ surface property modulation of liquid metal may provide promising prospects for efficient property tuning strategies and innovative on‐demand applications.