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2D conjugated metal‐organic frameworks (MOFs) with high in‐plane‐π‐conjugation are attracting significant attention in various fields owing to their outstanding electrical transport property, substantial specific surface areas, and tunable structures. However, their potential in ultrafast photonics has not been extensively explored. Herein, 2D conjugated Ni3(HITP)2 metal‐organic framework (MOF) and...