The use of radiometal complexes as radiopharmaceuticals for medical imaging is an area that is rapidly growing. Our interests are focused on the synthesis, characterization, and metal complexation of cross-bridged tetraamines and their ⁶⁴Cu, ^67,68Ga, and ¹¹¹In complexes. The complexation of Ga(III) with 1 via thermal heating has been challenging, thus microwave-assisted conditions have been explored to successfully complete the synthesis. In(III) complexation of 1 has also been problematic, though an indirect route involving alkylation of [In-CB-Cyclam]⁺ complex 2 to obtain synthetic intermediate 3 has been developed.