Since the discovery of graphene, two-dimensional materials with atomic thickness have attracted much attention because of their characteristic physical and chemical properties. Recently, coordination nanosheets (CONASHs) came into the world as new series of two-dimensional frameworks, which can show various functions based on metal complexes formed by numerous combinations of metal ions and ligands. This Feature Article provides an overview of recent progress in synthesizing CONASHs and in elucidating their intriguing electrical, sensing, and catalytic properties. We also review recent theoretical studies on the prediction of the unique electronic structures, magnetism, and catalytic ability of materials based on CONASHs. Future prospects for applying CONASHs to novel applications are also discussed.