We report the synthesis of hydrogen-bonded frameworks prepared from guanidinium, bis-amidinium or tetra-amidinium cations, and diphosphonate or tetraphosphonate anions. The frameworks are assembled by both charge-assisted amidinium⋅⋅⋅phosphonate and anti-electrostatic phosphonate⋅⋅⋅phosphonate hydrogen bonds, of which the phosphonate⋅⋅⋅phosphonate interactions are notably shorter. Frameworks prepared from the tetrahedral tetraphosphonate building block contain relatively... Show more