A convenient pathway for controlling defect-free nanoscopic domains large areas is illustrated. A simple rubbing technique is used to align nanocylinders self-assembled in an amphiphilic diblock liquid-crystalline copolymer by introducing novel supramolecular cooperative motions between mesogens and microphase domains. A 3D macroscopic array of the nanocylinders over a large area is achieved parallel to the rubbing direction (see figure and inside cover).