Molecular simulations for hydrogen physisorption with corannulene molecules arranged according to their crystal structure result in good agreement with the weight-percent hydrogen stored as determined experimentally employing a 3-g sample of highly crystalline corannulene at ambient temperatures and 72 bar of pressure. Calculated enthalpies of adsorption for corannulene/hydrogen molecular systems obtained from ab initio calculations which take into account electron correlation via second-order Moller-Plesset perturbation theory are in good agreement with literature experimental enthalpies of adsorption for activated carbons interacting with molecular hydrogen. Ab initio results also show that corannulene molecules arranged in a sandwich structure are important for approximately doubling the binding energy of corannulene interacting with molecular hydrogen through a cooperative interaction. To test the effects of finite temperatures and pressures, stack arrays were used as input for molecular dynamics simulations and indicate that physisorption mechanisms including van der Waals forces and dipole-induced dipole interactions may yield enhanced adsorption capacity in relation to other carbon-based materials. These results will be instrumental in identifying interlayer separations of an array of corannulene or related molecules that may provide a high weight percent of physisorbed hydrogen.