"(Figure Presented)" Narrow channels with polar walls are the structural and functional features responsible for the high capacity of a zinc-organic framework based on an imidazolate-amide-imidate ligand for the uptake of H₂ and CO₂ (see structure: orange Zn, blue N, red O, dark gray C, light gray H). The rigid and stable chelating ligand was synthesized in situ by partial hydrolysis of a dicyanoimidazole compound.