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The designed synthesis of a crystalline azulene‐based covalent organic framework (COF‐Azu‐TP) is presented and its photothermal property is investigated. Azulene, a distinctive 5–7 fused ring non‐benzenoid aromatic compound with a large intramolecular dipole moment and unique photophysical characteristics, is introduced as the key feature in COF‐Azu‐TP. The incorporation of azulene moiety imparts...