Carbide-derived carbons (CDCs) with specific surface area (SSA) ~ 2000 m2/g and open pore volume up to 80% are produced by chlorine etching of metal carbides. Tuning the pore size distribution by carbide precursor selection and etching temperature yields enhanced hydrogen storage capacity at both ambient and elevated pressure. Our goal is to establish the fundamental relation between capacity and SSA, pore size and pore volume.