The synthesis of nanoparticles has experienced a huge development over the past 20 years. However, this development has remained relatively limited to a few classes of nanomaterials such as iron oxides, semi-conducting oxides, plasmonic nanoparticles (essentially Au) and quantum dots. In these cases, a physical chemistry approach and standard recipes allow a good control of the size and shape of the resulting nano-objects. However, organometallic precursors have emerged as an important class allowing the preparation of a large variety of nano-objects, concerning a large number of elements and displaying a clean and controllable surface and therefore good physical and chemical properties. This perspective article is mostly devoted to the research efforts carried out by our group on the search for new classes of precursors and on the importance of knowing their exact structure and the molecular chemistry involved prior to the fabrication of the nano-objects.