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The introduction of a phenolate pendant arm in place of an acetate on AAZTA‐ and DATA‐like ligands resulted in hepta‐ and hexadentate chelators able to form Ga(III) complexes with thermodynamic stability and kinetic inertness higher than that of other Ga(III) complexes based on the parent 6‐amino‐6‐methylperhydro‐1,4‐diazepine scaffold. In particular, the heptadentate AAZ3A‐endoHB with a phenolate...