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In this work, nitrogen‐annulated perylene (NP) was dimerized into one framework connected by two nitrogen atoms, generating the target molecule of DNP−DA. Owing to the substructure of 1,6‐diazecine ten‐membered ring, DNP−DA illustrates helical chirality with moderate dissymmetry factor, elevated molecular levels, expanded conjugation and supramolecular interactions with acceptors etc. Notably, DNP−DA...