Over a period of many decades, the chemistry of metal–carbon bonds has given rise to an ever-growing field of fundamental research and applied science, merging the reactivity of inorganic complexes with the structural diversity of organic compounds. The contributions in this Thematic Series reflect the broad impact of organometallic compounds in various fields of modern chemical research. These include the tailoring of new ancillary ligands, the investigation of more active and more selective homogeneous catalysts, catalytic transformations in the total synthesis of natural products, the theoretical and kinetic unravelling of reaction mechanisms, and the verification of rare coordination modes. These various facets underline the importance of organometallic chemistry in its own right, but also demonstrate the vital role that research in organometallic chemistry plays as a provider of invaluable tools for other chemistry sub-disciplines.