Metal-organic frameworks (MOFs) with open metal sites exhibit a much stronger H2 binding strength than classical MOFs, due to the direct interaction between H2 and the coordinately unsaturated metal ions. Here we report a systematic study of the H2 adsorption on a series of isostructural MOFs, M2(dhtp) (M = Mg, Mn, Co, Ni, Zn). The experimental, initial isosteric heats of adsorption for H2 (Qst) of these MOFs range from 8.5 to 12.9 kJ/mol, with increasing Qst in the following order: Zn, Mn, Mg, Co, and Ni. The H2 binding energies derived from first-principles calculation follow the same trend as the experimental observation on Qst, confirming the electrostatic Coulomb attraction between the H2 and the open metals being the major interaction. We also found a strong correlation between the metal ion radius, the M-H2 distance, and the H2 binding strength, which provides a viable, empirical method to predict the relative H2 binding strength of different open metals.