Lewis base-free lanthanoid (Ln) and actinoid (An) iodides are difficult to obtain, as standard protocols describe syntheses in solutions of donor solvents which are ultimately hard to remove. We have now established a mechanochemical approach towards the synthesis of Lewis base-free f-block metal iodides with excellent yields. In particular, we describe herein the synthesis of EuI2 as an example of a divalent lanthanoid iodide, of CeI3 as an example of a trivalent lanthanoid iodide, and of UI3 as the most important actinoid iodide. Each can be obtained in high yield with minimal work-up, presenting the most efficient and simple synthetic route to access these materials to date.