Widespread use of hydrogen as an energy carrier is a key priority for the EU, in order to achieve its climate and energy transition targets. Developing sustainable, efficient and safe hydrogen storage technologies has, however, proved challenging. MOST-H2, in full alignment with the requirements of HORIZON-CL4-2021-RESILIENCE-01-17, proposes an integrated multiscale lab-to-tank approach to develop, validate and demonstrate innovative, low cost cryo-adsorptive hydrogen storage, using monolithic Metal-Organic Framework (MOF) adsorbents, with an optimal combination of volumetric and gravimetric capacity, but also a small environmental footprint. Advanced synthetic strategies and sophisticated computational techniques, including molecular simulation and machine learning, will be combined in a cyclic materials development approach, to deliver new high performance, sustainable-by-design MOF adsorbents. The main aim is to computationally design, then synthesise and validate experimentally, ultra porous MOFs with usable storage capacities above 10 wt% and 50 g/L on a materials basis, at an operating pressure below 100 bar. This represents an essential step towards more efficient, intrinsically safer and cost effective storage solutions, compared to conventional hydrogen storage technologies. An important part of the project will be devoted to developing and upscaling monolithic forms of optimal MOF materials to allow easy integration into a cryo-adsorption storage tank, specifically designed for this purpose, which will be tested in a TRL 5 environment. The outcomes, coupled with full life cycle analysis and techno-economic assessment of MOST-H2 technology, with a view to selected end uses (rail and road applications), will form the basis for elaborating future market penetration plans through a solid horizontal dissemination and exploitation strategy.