At the dawn of the development of structural organometallic chemistry, soon after the discovery of ferrocene, the description of the LnCp3 complexes, featuring large and mostly trivalent lanthanide ions, was rather original and sparked curiosity. Yet, the interest in these new architectures rapidly dwindled due to the electrostatic nature of the bonding between π-aromatic ligands and 4f-elements. Almost 70 years later, it is interesting to focus on how the discipline has evolved in various directions with the reports of multiple catalytic reactivities, remarkable potential in small molecule activation, and the development of rich redox chemistry. Aside from chemical reactivity, a better understanding of their singular electronic nature – not precisely as simplistic as anticipated – has been crucial for developing tailored compounds with adapted magnetic anisotropy or high fluorescence properties that have witnessed significant popularity in recent years. Future developments shall greatly benefit from the detailed reactivity, structural and physical chemistry studies, particularly in photochemistry, electro- or photoelectrocatalysis of inert small molecules, and manipulating the spins' coherence in quantum technology.