Extensive research has been carried out in the field of materials-based H2 storage during the last two decades, where nanoporous and high-surface area carbons are studied as efficient sorbent materials for physical adsorption and confinement of H2 inside their porous structure. However, these carbons are usually produced as loose and fine powders, thus creating technical issues regarding their safe handling and large-scale implementation in H2 storage systems for stationary and mobile applications. Herein, a pure carbon material in cloth-like form, with large specific surface area (~1200 m2/g) and pore volume (~0.5 cm3/g) as well as narrow ultra-micropore sizes (~0.6 nm), was produced via carbonization and CO2 activation of a cellulose-based polymer (viscose rayon cloth). The H2 cryo-adsorption behavior was fully reversible at temperatures below 100 K and a significant H2 gravimetric uptake of ~3.10 wt.% was recorded at 77 K and ~60 bar. However, the equivalent performance at 298 K was rather poor (< 0.2 wt.%) and not sufficient for practical applications. Therefore, the carbon cloth material was doped with magnetron sputter deposited Pd with the intention to enhance the carbon surface-molecular H2 interaction at room temperature. The outcome of this novel approach is discussed in detail.