Nanosheet materials have attracted significant attention because of their unique electronic and physical properties, which derive from their two-dimensional (2D) nature. Graphene and other 2D inorganic sheet assemblies of metal chalcogenides are prominent nanosheet materials which are widely exploited in electronics, photonics, and spintronics technologies, because 2D materials possess close affinity with those used in the silicon-based electronics. Most of these nanosheets have been synthesized via exfoliation of bulk layered materials, which is a top-down method. In contrast, “bottom-up” nanosheets are generally synthesized directly from organic compounds, ligands, and/or metal ion connectors, and their composition, structure, and properties can be tuned at will by tailoring the constituent components used. This is a strong point of using bottom-up nanosheet against the top-down congener. However, application studies of the bottom-up 2D metal-complex nanosheets are still very rare. In this lecture, the bottom-up synthesis of some functional 2D metal complex nanosheets from molecular precursors will be presented which can be monometallic or bimetallic in nature. Both single-layer and multilayer 2D nanosheets will be developed depending on the fabrication method (i.e. gas-liquid or liquid-liquid interfacial synthesis). The ligand structure can be easily altered in terms of the spacer group and the number of arms. The metal complexes can be modified to show significant π-conjugation and intense absorptions in the visible and near-infrared region, which will be useful for the construction of photoresponsive and semiconductive nanosheets. The resulting nanosheets are shown to find wide applications in optoelectronics and catalysis.