This communication reports a shape-controlled synthesis of colloidal superparticles (SPs) from iron oxide nanocubes. Our results show that the formation of SPs is under thermodynamic control and that their shape is determined by Gibbs free energy minimization. The resulting SPs adopt a simple-cubic superlattice structure, and their shape can be tuned between spheres and cubes by varying the relative free energy contributions from the surface and bulk free energy terms. The formation of sphere-shaped SPs from nanocubes suggests that the size-dependent hydration effect predicted by the Lum-Chandler-Weeks theory plays a very important role in the self-assembly of nano-objects. In addition, the iron oxide SPs exhibit shape-dependent therapeutic effects in magnetomechanical treatments of cancer cells in vitro.