Mononuclear metal complexes, particularly those based on platinum and ruthenium metal centers, have attracted tremendous attention over recent decades for therapeutic purposes, particular anticancer therapy. However, inorganic architectures based on supramolecular coordination complexes (SCCs) have received comparatively less attention for biological applications. In this chapter, we highlight recent examples of SCCs that interact with DNA or protein through different binding modes and/or exhibit cytotoxic activity against cancer cell lines.