Metal-organic frameworks (MOFs) are permanently porous, crystalline materials and promising hydrogen sorbents. However, the H2 heats of adsorption are generally too small to promote significant adsorption under desired storage conditions. Increasing the H2-framework interaction energy is a prominent goal of current MOF design. Hydrogen binds to MOFs through a variety of interactions, such as dispersion, charge-induced-dipole, charge-quadrupole, and even chemical bonding. To date, these interactions have been enhanced by incorporating strongly charged groups into the MOF structures, but the effects tend to be short-range and only effective at low loadings. In this work we report the structures and H2 storage properties of two zwitterionic MOFs. These structures feature zwitterionic characteristics arising from N-heterocyclic azolium groups in the linkers and negatively charged Zn2(CO2)5 nodes. These groups exhibit net charges of +0.5 and -1.0, respectively, and interact strongly with the H 2 quadrupole. Isosteric heats of adsorption of up to 7.0 kJ mol -1 are observed in these zwitterionic MOFs.