© 2015 American Chemical Society. Despite their wide utility in laboratory synthesis and industrial fabrication, gas-water-solid multiphase catalysis reactions often suffer from low reaction efficiency because of the low solubility of gases in water. Using a surface-modification protocol, interface-active silica nanoparticles were synthesized. Such nanoparticles can assemble at the gas-water interface, stabilizing micrometer-sized gas bubbles in water, and disassemble by tuning of the aqueous phase pH. The ability to stabilize gas microbubbles can be finely tuned through variation of the surface-modification protocol. As proof of this concept, Pd and Au were deposited on these silica nanoparticles, leading to interface-active catalysts for aqueous hydrogenation and oxidation, respectively. With such catalysts, conventional gas-water-solid multiphase reactions can be transformed to H 2 or O 2 microbubble reaction systems. The resultant microbubble reaction systems exhibit significant catalysis efficiency enhancement effects compared with conventional multiphase reactions. The significant improvement is attributed to the pronounced increase in reaction interface area that allows for the direct contact of gas, water, and solid phases. At the end of reaction, the microbubbles can be removed from the reaction systems through changing the pH, allowing product separation and catalyst recycling. Interestingly, the alcohol oxidation activation energy for the microbubble systems is much lower than that for the conventional multiphase reaction, also indicating that the developed microbubble system may be a valuable platform to design innovative multiphase catalysis reactions.