Self-organization of colloidal Pt nanocubes into two types of distinct ordered superlattices, simple-cubic and body-centered-tetragonal structures, has been achieved using a home-built setup. Detailed translational and orientational characteristics of these superstructures were determined using a transmission electron microscopy tomographic technique with 3D reconstruction analysis. The formation of these distinct superlattices is the result of a delicate choice of solvent (i.e., aliphatic hexane or aromatic toluene hydrocarbons), which serves as a dispersion medium to fine-tune the relative strengths of ligand-ligand and ligand-solvent interactions during the self-assembly process. This work provides important insights into the effects of ligand-solvent interactions on superlattice formation from nonspherical nanoparticles.