Biological waste such as residues from the food and beverage industry provides a valuable and abundant resource to be used as a precursor for the synthesis of activated carbons that can be subsequently employed as adsorbents for, e.g., hydrogen storage. Materials with a large specific surface area and pores of appropriate size are necessary to achieve reasonable hydrogen adsorption capacity. Here, we present the repeatable synthesis of activated carbons from coffee waste, i.e., spent coffee grounds and coffee silver skins, on the basis of two independently synthesized batches. The carbonization process under nitrogen gas flow followed by chemical activation with solid potassium hydroxide results in microporous carbons with bimodal pore size distribution and specific surface area up to 3300 and 2680 m2/g based on Brunauer–Emmett–Teller and density functional theory methods, respectively. The materials exhibit excellent hydrogen adsorption performance under cryogenic conditions (77 K), reaching high and fully reversible excess gravimetric hydrogen uptake values of up to 5.79 wt % at 37 bar, and total capacities exceeding 9 wt % at 100 bar.