The synthesis of layered double hydroxides (LDHs) provides a relatively easy and traditional way to build versatile chemical compounds with a rough control of the bulk structure. The delamination of LDHs to form their single host layers (2D nanosheets) and the capability to reassemble them offer the possibility to gain precise control of the structure, composition, morphology, and property of desired nanostructures. In the present Ph.D. project, examples to produce 2D nanosheets with novel functionalities are presented. This comprises: (1) Synthesis of LDHs with a new structure and composition. (2) Delamination of the LDHs structure (oxGRC12) with the formation of single sheet iron (hydr)oxide (SSI). (3) Assembly of the new 2D nanosheets layer by layer to achieve desired functionalities.