Electron microscopy methods have been used to visualize individual spherical and cylindrical supramolecular dendrimers, providing definitive confirmation of the structures suggested by previous x-ray diffraction analysis that assumed a microsegregated model. These dendrimers are self-assembled, self-organized, and aligned spontaneously and simultaneously in hexagonal columnar or cubic thermotropic liquid-crystal phases with high uniformity. Homeotropic and planar ordering of the hexagonal columnar liquid crystal was precisely controlled by a variety of surfaces. The stiffness of these cylinders was evaluated by examining their planar texture and its defects.