Open and close: Inspired by close‐packing of spheres, to strengthen the framework–H2 interaction in MOFs (metal‐organic frameworks), a strategy is devised to increase the number of nearest neighboring open metal sites of each H2‐hosting cage, and to align the open metal sites toward the H2 molecules. Two MOF polymorphs were made, one exhibiting a record high hydrogen uptake of 3.0 wt % at 1 bar and 77 K.