The ammonium-based OSDAs with a various chemical properties (Supplementary Table ) form different types of intermolecular interactions with the host MOF frameworks. All OSDAs are charge-balancing cations that have coulombic (electrostatic) interactions with the anionic frameworks where the anionic sites are deprotonated phenolate oxygen atoms. In all as-synthesized MOF structures except SU-111, the OSDAs are hydrogen-bond donors and interact with the frameworks through hydrogen bonds between the nitrogen atoms of ammonium sites and various hydrogen-bond accepting oxygen atoms of the ellagate ligands. In one ellagic acid molecule, there are two phenol oxygen atoms from catechol groups located at both the para (1) and meta (2) positions of the biaryl C-C bond, as well as two different types of oxygen atoms in lactones, an ether (3) and a carbonyl (4) oxygen. These four different types of oxygen atoms are marked with their numerical codes in Fig. . The various OSDAs form hydrogen bonds to different ellagate oxygen atoms in the MOFs. As hydrogen atoms are difficult to locate directly from experimental 3D ED data, we interpret donor-acceptor distances ≤ 3.3 Å as hydrogen bonds.