Abstractvan der Waals heterostructures formed by 2D materials have attracted much attention in the last few years. Recently, 2D nanosheets linked by covalent bonds have been found to exhibit novel properties. In the present study we have investigated supramolecular layered heterostructures formed by nanosheets of MoS2 with BC7N, g‐C3N4 and graphene. These materials have been synthesized via a non‐covalent host–guest synthetic design using cucurbit[8]uril (CB[8]) hosts. In addition to offering reversible disassembly, these heterostructures show good visible‐light‐driven hydrogen evolution reaction (HER) activity as well as reasonable gas adsorption and other properties.
