Metal-organic frameworks (MOFs) are promising materials for onboard hydrogen storage thanks to the tunable pore size, pore volume, and pore geometry. In consideration of pore structures, the correlation between the pore volume and hydrogen storage capacity is examined and two empirical equations are rationalized to predict the hydrogen storage capacity of MOFs with different pore geometries. The total hydrogen adsorption under 100 bar and 77 K is predicted as ntot = 0.085× Vp - 0.013× Vp 2 for cage-type MOFs and ntot = 0.076× Vp - 0.011× Vp 2 for channel-type MOFs, where Vp is the pore volume of corresponding MOFs. The predictions by these empirical equations are validated by several MOFs with an average deviation of 5.4%. Compared with a previous equation for activated carbon materials, the empirical equations demonstrate superior accuracy especially for MOFs with high surface area (i.e., SBET over ≈3000 m2 g-1 ). Guided by these empirical equations, a highly porous Zr-MOF NPF-200 (NPF: Nebraska Porous Framework) is examined to possess outstanding hydrogen total adsorption capacity (65.7 mmol g-1 ) at 77 K and record high volumetric working capacity of 37.2 g L-1 between 100 and 5 bar at 77 K.