Hydrazine, monomethylhydrazine, and ethylenediamine react readily and reversibly with carbon dioxide to form hydrazinium carboxylate, monomethylhydrazinium carboxylate, and ammonium carbamate adducts, respectively. These adducts act as low molecular weight gelators, which self-assemble and in doing so trap unreacted hydrazine or diamine. The properties and molecular structures of the gels were investigated by means of elemental analysis, DSC/TGA, heteronuclear NMR (H-1, N-15, and C-13), diffusion-ordered NMR spectroscopy (DOSY), and cryo-immobilized high resolution scanning electron microscopy (cryo-HRSEM). These complementary techniques provided the foundation for developing a pictorial representation of the bulk gel structures on the molecular level.