Self-organized supramolecular organic nanostructures have potential applications that include molecular electronics, photonics, and precursors for nanoporous catalysts. Accordingly, understanding how self-assembly is controlled by molecular architecture will enable the design of increasingly complex structures. We report a liquid crystal (LC) phase with a tetragonal three-dimensional unit cell containing 30 globular supramolecular dendrimers, each of which is self-assembled from 12 dendron (tree-like) molecules, for the compounds described here. The present structure is one of the most complex LC phases yet discovered. A model explaining how spatial arrangement of self-assembled dendritic aggregates depends on molecular architecture and temperature is proposed.