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Thick photosensitive films with sufficient light penetration are required for improving the capacity of recording media based on azopolymers. Block copolymers having an azo liquid crystalline block allow the dilution of azo chromophores but maintain the cooperativity among them. On page 1716, Jesús del Barrio, Eva Blasco, Luis Oriol, Rafael Alcalá, and Carlos Sánchez-Somolinos describe the self-assembly of azo chromophores and pyridine units of commercial polystyrene-b-poly(4-vinylpyridine)s to obtain photoresponsive supramolecular block copolymers. This approach offers a versatile and facile method for the preparation of photoresponsive block copolymers for volume holographic storage.