Hydrogen gas (H₂) is a clean and renewable energy source, but the lack of efficient and cost-effective storage materials is a challenge to its widespread use. Metal–organic frameworks (MOFs), a class of porous materials, have been extensively studied for H₂ storage due to their tunable structural and chemical features. However, the large design space offered by MOFs makes it challenging to select or design appropriate MOFs with a high H₂ storage capacity. To overcome these challenges, we present a data-driven computational approach that systematically designs new functionalized MOFs for H₂ storage. In particular, we showcase the framework of a hybrid particle swarm optimization integrated genetic algorithm, grand canonical Monte Carlo (GCMC) simulations, and our in-house MOF structure generation code to design new MOFs with excellent H₂ uptake. This automated, data driven framework adds appropriate functional groups to IRMOF-10 to improve its H₂ adsorption capacity. A detailed analysis of the top selected MOFs, their adsorption isotherms, and MOF design rules to enhance H₂ adsorption are presented. We found a functionalized IRMOF-10 with an enhanced H₂ adsorption increased by ∼6 times compared to that of pure IRMOF-10 at 1 bar and 77 K. Furthermore, this study also utilizes machine learning and deep learning techniques to analyze a large data set of MOF structures and properties, in order to identify the key factors that influence hydrogen adsorption. The proof-of-concept that uses a machine learning/deep learning approach to predict hydrogen adsorption based on the identified structural and chemical properties of the MOF is demonstrated.