The development of novel materials capable of securely storing hydrogen at high volumetric and gravimetric densities is a requirement for the wide-scale usage of hydrogen as an energy carrier. In recent years, great efforts via nanoscale tuning and designing strategies on both physisorbents and chemisorbents have been devoted to improvements in their thermodynamic and kinetic aspects. Increasing the hydrogen storage capacity/density for physisorbents and chemisorbents and improving the dehydrogenation kinetics of hydrides are still considered a challenge. The extensive and fast development of advanced nanotechnologies has fueled a surge in research that presents huge potential in designing solid-state materials to meet the ultimate U.S. Department of Energy capacity targets for onboard light-duty vehicles, material-handling equipments, and portable power applications. Different from the existing literature, in this review, particular attention is paid to the recent advances in nanoscale engineering of solid-state materials for boosting hydrogen storage, especially the nanoscale tuning and designing strategies. We first present a short overview of hydrogen storage mechanisms of nanoscale engineering for boosted hydrogen storage performance on solid-state materials, for example, hydrogen spillover, nanopump effect, nanosize effect, nanocatalysis, and other non-classical hydrogen storage mechanisms. Then, the focus is on recent advancements in nanoscale engineering strategies aimed at enhancing the gravimetric hydrogen storage capacity of porous materials, reducing dehydrogenation temperature and improving reaction kinetics and reversibility of hydrogen desorption/absorption for metal hydrides. Effective nanoscale tuning strategies for enhancing the hydrogen storage performance of porous materials include optimizing surface area and pore volume, fine-tuning nanopore sizes, introducing nanostructure doping, and crafting nanoarchitecture and nanohybrid materials. For metal hydrides, successful strategies involve nanoconfinement, nanosizing, and the incorporation of nanocatalysts. This review further addresses the points to future research directions in the hope of ushering in the practical applications of hydrogen storage materials.