Since the first intercalation of layered silicates by using supercritical CO2 as a processing medium, considerable efforts have been dedicated to intercalating and exfoliating layered two‐dimensional (2D) materials in various supercritical fluids (SCFs) to yield single‐ and few‐layer nanosheets. Here, recent work in this area is highlighted. Motivating factors for enhancing exfoliation efficiency and product quality in SCFs, mechanisms for exfoliation and dispersion in SCFs, as well as general metrics applied to assess quality and processability of exfoliated 2D materials are critically discussed. Further, advances in formation and application of 2D material–based composites with assistance from SCFs are presented. These discussions address chemical transformations accompanying SCF processing such as doping, covalent surface modification, and heterostructure formation. Promising features, challenges, and routes to expanding SCF processing techniques are described.