In the field of interfacial science, the formation, maintenance and rupture theory of bubble gas-liquid two-phase interface has been an important basic scientific issue. Compared to soapy water, it is impossible to blow bubbles only with pure water since the interaction between water molecules is too strong, making it more inclined to form water droplets. The addition of soap makes it easier to form and maintain bubbles. However, even with the help of surfactants, beautiful soap bubbles are fleeting and rather easily destroyed. This is because the bubble is a thermodynamically unstable system with a high surface Gibbs function. [4] When the bubble is formed, the gas-liquid interface area and the interfacial free energy of the system increases. Therefore, the formation of bubbles is a thermodynamically nonspontaneous process that requires external work on the system. Overall, the addition of surfactants can reduce the gas-liquid interfacial tension, thus reducing the energy consumption when blowing bubbles, which is beneficial to the formation and stability of bubbles. [5] In addition, the more important role of the surfactant lies in that its molecules can form an oriented monolayer on the gas-liquid interface, with the polar end points to the water. The more tightly the surfactants are arranged on the fluid surface, the firmer the interfacial film and the more stable the bubbles.Water is usually adopted in traditional bubble studies because of its inherently low surface tension (≈70 mN m −1 ) and the ability of surfactants to further reduce the surface tension. While in this work, we propose to introduce a high-surface-tension liquid metal (LM) fluid and study the formation of membrane structure in a solution (S) environment. Among the many possible LM candidates, gallium-based low-melting-point LM has received extensive attention in recent years, since it combines the virtues of liquid, such as fluidity, flexibility, and deformability with the advantages of metals, like high electrical conductivity and heat conductivity. [6] Besides, gallium-based alloys are nontoxic and all components have a very low vapor pressure at elevated temperature, which permits safe handling. [7] Owing to these outstanding merits, LM is believed to be an alternative material to realize numerous functions and has therefore been applied in a variety of significant areas, [8][9][10] including device cooling, flexible electronics, deformable antennas, biomedical technology, 3D print, etc. Besides, LM has been found to display a wealth of surface and interface phenomena since such a Conventional bubbles are generally made of an outside water film and the interior air, and their formation and rupture involve rich scientific knowledge. An intriguing question is what would happen if the water film and air of such bubbles were replaced by completely different fluids? Here, a high-surfacetension liquid metal-solution bilayer is introduced into the two-phase interface system, and a new conceptual hybrid vacuole consisting of a liquid metal outer...