Layered inorganic solids as an attractive classification of 2D materials offer material diversity and a wide range of interesting properties. Layered inorganic solids provide an expandable 2D nanospace between each individual layer, the so called interlayer space, to accommodate/arrange guest species such as molecules, nanoparticles, and polymer chains and design unique nanoarchitectures, resulting in the production of intercalation compounds showing different properties in comparison to those of virgin layered materials and guest species. Layered inorganic solids can also be exfoliated to result in nanosheet production. Further ordering of exfoliated nanosheets is also possible via different methods and normally leads to creating soft materials presenting properties and applications different from that of relatively rigid intercalation compounds. Here, the latest studies and up-to-date developments on the possible techniques of designing novel types of materials using layered inorganic solids are specifically highlighted.