Ab initio studies on molecular hydrogen adsorption in lithium-doped hexaborane(6) (B₆H₆Li₂) have been carried out. Our calculated results show that the lithium sites in the complex carry a partial positive charge, and the binding energy of Li to the borane framework, as calculated at the MP2/aug-cc-pVTZ level of theory, is found to be -196.467 kcal/mol per lithium, which is large enough to ensure the stability toward recyclability. This charged surface created around the metal atom is found to interact with molecular hydrogen through charge induced dipole interaction. Each lithium site is found to adsorb a maximum of three hydrogen molecules which corresponds to a gravimetric density of 12 wt %. We have also verified the possibility of constructing a three-dimensional solid using the dilithium-doped B6 unit as a building block and -CtC- units as a linking agent. The hydrogen adsorption properties of this designed structure show that it can adsorb hydrogen with a gravimetric density of 7.3 wt %, and binding energy per molecular hydrogen is found to be around -2.2 kcal/mol.