In today's world, where environmental concerns are growing and human impact on climate change is undeniable, shifting from traditional fossil fuels to renewable energy sources has become not just a preference but an essential need. Exploring efficient and sustainable approaches to store and transport environmentally benign fuel sources is becoming crucial. We now face the reality that our historical reliance on hydrocarbons extracted from below the ground is unsustainable and ecologically harmful. In turn, hydrogen, with its energy stored in H-H bonds, is a promising energy carrier since its use in either fuel cells or even combustion is itself harmless to the environment, yielding only water as a chemical byproduct. As a specific example involving an economically vital application, adapting heavy-duty transport to run on hydrogen fuel is an attractive, eco-friendly solution. However, moving towards a hydrogen-based economy brings several challenges. Physical-based storage of hydrogen typically requires either extremely high pressures (350-700 bar) or very low, cryogenic temperatures for hydrogen liquefaction (-252.8 °C at 1 atm). These processes consume a lot of energy, both for compressing the hydrogen and maintaining low temperatures. Additionally, storing highly flammable gas under more than 350 bar pressure raises risk concerns, especially in the context of daily transportation, while boil off from liquid hydrogen can lead to significant losses for longer periods of storage. A promising approach for hydrogen storage at moderate pressures is through the use of adsorbents. In this context, metal-organic frameworks (MOFs) present a potentially ideal solution. The most promising materials still mostly rely on cryogenic temperatures for peak effectiveness, lowering the energy efficiency. However, MOFs have remarkable synthetic flexibility, allowing for the fine-tuning of a broad spectrum of physical properties. This range extends from adjusting pore sizes and surface areas to modifying the coordination geometry of the transition metal sites. Nonetheless, systematic experimental exploration of each MOF from the extensive list of potential combinations presents challenges in terms of both time and resources. It is clear that there is still a great range of unexplored materials that can potentially offer improved performance. In turn, computational modeling offers guidance in identifying and evaluating the most promising MOF candidates for efficient hydrogen storage without synthesizing the materials, which sometimes requires months or even more than a year of human effort. Furthermore, theory could offer insights into the electronic structure of the material, providing further pathways for subsequent optimizations. Although MOFs are well-known for their porosity, the strategy for optimizing a MOF for hydrogen storage must go beyond merely increasing its surface area. While it is true that the gravimetric uptake of hydrogen increases with greater surface area, the volumetric uptake, crucially important for hydrogenfueled transportation, decreases. In addition, relying solely on weak physisorption, characterized by binding enthalpies around -5 kJ/mol, is inadequate for attaining substantial usable capacities at room temperature and results in unsatisfactorily low hydrogen densities. A clear illustration of this can be seen with the MOF-5 (Zn4O(bdc)3; bdc 2-= benzene-1,4-dicarboxylate) material, which exhibits relatively high surface areas (BET surface areas of 3800 m 2 /g) among MOFs and was the first MOF that was studied for hydrogen storage. MOF-5 demonstrates a volumetric H2 capacity of 63 g/L at 77 K and 80 bar, but only 8.9 g/L at room temperature and 100 bar. The hydrogen uptake of 8.9 g/L is significantly lower than the 39.8 g/L achieved with compressed H2 at room temperature and 700 bar, rendering it insufficient for competitive applications in transportation.