Hydrogen adsorption on crystalline ropes of carbon single-walled nanotubes ͑SWNT͒ was found to exceed 8 wt. %, which is the highest capacity of any carbon material. Hydrogen is first adsorbed on the outer surfaces of the crystalline ropes. At pressures higher than about 40 bar at 80 K, however, a phase transition occurs where there is a separation of the individual SWNTs, and hydrogen is physisorbed on their exposed surfaces. The pressure of this phase transition provides a tube-tube cohesive energy for much of the material of 5 meV/C atom. This small cohesive energy is affected strongly by the quality of crystalline order in the ropes.