Abstract

Abstract There is a strong desire to design and synthesize catalysts that assemble at the oil–water interface to improve the efficiency of biphasic reactions. Anisotropic dumbbell‐shaped bi‐component mesoporous carbon–organosilica Janus particles with asymmetric wettability are synthesized through a one‐step compartmentalized growth of a mesoporous organosilica sphere attached to a mesoporous resorcinol–formaldehyde (RF) sphere. A library was prepared of tunable Janus particles possessing diverse hollow structures with various functionalities. As a proof of concept, the Janus particle‐derived catalyst can assemble at the oil–water interface to stabilize Pickering emulsions. Owing to the increased reaction interface area, the Janus catalyst exhibits a more than three‐fold increase in catalytic efficiency compared to the Pt loaded carbon sphere catalyst in aqueous hydrogenation reactions.