The highly stable CTi72+ cluster recently theoretical predicted (J. Phys. Chem. Lett. 2012, 3, 2264) were investigated as a candidate for hydrogen storage material within DFT framework. The covalent interactions stemming from strong orbital overlaps between C-2p and Ti-3d (4s) was revealed by QTAIM and DOS analyses. The CTi72+ cluster can bind 20 H-2 molecules at most, which can result into the gravimetric density of 19%. The interaction energies between H2 molecules and CTi72+ cluster are in the range of 0.24-0.31 eV at B3LYP level of theory, and these energies are about 0.1 eV larger when long range interaction was considered with wB97xD and CAM-B3LYP functionals. The binding energies for the present systems meet the thermodynamic requirement for reversible hydrogen reaction. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.