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.

By grafting an N-heterocyclic carbene palladium complex and ionic liquid on the mesoporous cage-like material SBA-16, an efficient and highly recyclable heterogeneous catalyst for the Suzuki and Heck reactions was prepared. This catalyst afforded a fast conversion of the unactivated bromobenzene at a catalyst loading of 0.01 mol%, and a good yield was still achieved after the catalyst was reused ten times. Its recyclability was much better than that of the catalyst prepared from amorphous silica. The significantly enhanced recyclability could be attributed to the isolated nanocages of SBA-16 which could efficiently prevent the aggregation and agglomeration of Pd particles formed during the catalytic reaction into the less active large particles. The strategy for stabilizing metal nanoparticles using the isolated nanocages may be applied to other catalytic systems, in which the aggregation of metal nanoparticles is desired to be prevented.