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The expanded phthalocyanine (EPc) single‐layer sheets with embedded double transition metals (labeled as TM2EPc) are predicted to be a novel class of highly stable 2D materials with a series of fascinating properties by means of systematic first‐principles calculations, molecular dynamics, and Monte Carlo simulations. Excitingly, the ferromagnetic Cr2EPc and antiferromagnetic Mn2– and Fe2–EPc have...