The development of hydrogen technologies and a wider use of hydrogen fuel cell systems require new materials that can store large amounts of hydrogen at relatively low pressures with small volume, low weight, and fast kinetics for recharging. Among the most challenging materials for hydrogen storage are porous coordination polymers, also called metal–organic frameworks (MOFs). MOFs are two- or three-dimensional porous crystalline materials with infinite lattices. As a result of their ultra-high surface area values (more than 2500 m2·g–1 measured by the Brunauer–Emmett–Teller (BET) approach), they were found to be promising gas adsorbers for small gaseous molecules, including CH4, CHCl3, CCl4, C6H6, C6H12, CO2, Ar, N2, and H2. The main benefit of MOFs is their reversible and high-rate hydrogen adsorption process. A reasonable number of H2 molecules inside the body of MOFs may only be obtained at very low temperatures. To date, MOFs have shown significant progress in applications of gas separation, catalysis, and coordination chemistry.