Hydrogen storage capacity, stability, bonding mechanism, and the electronic structure of polylithiated molecules (OLi2) functionalized graphane (CH) has been studied by means of first principle DFT. Molecular dynamics have confirmed the stability, while Bader charge analysis describes the bonding mechanism of OLi2 with CH. The binding energy of OLi2 on CH sheet has been found to be large enough to ensure its uniform distribution without any clustering. It has been found that each OLi2 unit can adsorb up to six H2 molecules resulting into a storage capacity of 12.90wt. % with adsorption energies within the range of practical H2 storage application. © 2012 American Institute of Physics.