Two monoamide derivatives of 1,4,7-triazacyclononane-1,4,7-triacetic acid (NOTA) conjugated with methylamine (4) or benzylamine (5) were synthesized by treating di-tert-butyl 1,4,7-triazacyclononane-1,4-diacetate (1) with 2-chloro-Nbenzyl-or -N-methylacetamide, followed by an acid cleavage reaction. Complexes of 4 and 5 chelated to Ga 3+ to give Ga-4 and Ga-5, respectively, in reaction solutions at different pH values (3 and 5). Complexes Ga-4 and Ga-5 were characterized by single-crystal X-ray diffraction and multinuclear NMR spectroscopy. In the solid state, these complexes were isostructural, and the coordination spheres of the metal ions exhibited distorted octahedral geometries. In the case of the Ga-4 complex, which was formed at both pH values, the metal ion is coordinated to the amide nitrogen atom of the modified pendent arm of 4. However, in the case of Ga-5, the metal ion is coordinated to a nitrogen or an oxygen atom of the amide linkage when the pH of the reaction soultion was