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The azafullerene Tb 2 @C 79 N is found to be a single‐molecule magnet with a high 100‐s blocking temperature of magnetization of 24 K and large coercivity. Tb magnetic moments with an easy‐axis single‐ion magnetic anisotropy are strongly coupled by the unpaired spin of the single‐electron Tb−Tb bond. Relaxation of magnetization in Tb 2 @C 79 N below 15 K proceeds via quantum tunneling of magnetization with the characteristic time  τ  QTM =16 462±1230 s. At higher temperature, relaxation follows the Orbach mechanism with a barrier of 757±4 K, corresponding to the excited states, in which one of the Tb spins is flipped.

High Blocking Temperature of Magnetization and Giant Coercivity in the Azafullerene Tb 2 @C 79 N with a Single‐Electron Terbium–Terbium Bond