Ultrastrong metallic alloys, possessing unparalleled load-bearing abilities, are coveted in many sectors, thus attracting growing research efforts. However, these alloys encounter persistent usability challenges posed by hydrogen embrittlement, which causes unpredictable fracture through crack initiation. Due to complex hydrogen-microstructure interactions and their exacerbation under high stress, advances in hydrogen resistance in ultrastrong materials are sparse throughout their long history. Herein, we report a quantum-mechanics-informed strategy for hydrogen tolerance enhancement in ultrafine-grain-hardened Al-Zn-Mg-Cu alloys, approaching their current strength limit of approximately 1 GPa. This method involves the incorporation of hydrogen-absorbing T-phase precipitates into nanograins, to substantially reduce hydrogen coverage at potential crack initiation sites. We demonstrate, via synchrotron radiation X-ray micro-/nano-tomography, scanning transmission electron microscopy and atom probe tomography, that nanoprecipitates successfully withstand shear strains exceeding 1000 and are exploitable essentials for ultra strength-hydrogen synergy, contrasting their often-assumed secondary roles in nanocrystalline alloys due to possible strain-induced dissolution, which has intuitively excluded exploring them as central elements. Our approach potentially inspires new hydrogen-resisting alloys across a broad strength-composition space.