Layered materials held together by weak interactions can be exfoliated into monolayers that retain the structure and composition of their bulk counterpart, but this has remained challenging to achieve for non-van der Waals materials. Now, AgCrS2 has been exfoliated into such [CrS2]Ag[CrS2] nanosheets through intercalation with tetraalkylammonium cations chosen for their suitable redox potential. The nanosheets show superionic behaviour at room temperature.