This study is dedicated to the memory of Leone Spiccia, who would have loved to see the chromium Keggin ion finally come to fruition.Abstract: Aqueous metal-oxo clusters without organic ligands (including polyoxometalates and group 13 polycations) are useful for energy, environmental and biomolecular applications. While ligands stabilize clusters of different elements, such as open-shell transition metals, they inhibit reactivity and solubility. Therefore a grand challenge is to conceive and execute synthetic strategies to isolate metal-oxo clusters of any composition, without ligation. Here we crystallize and structurally characterize a Cr 3+ dodecamer Keggin ion without organic ligation.[a]