The structures and hydrogen storage capacities of B6Ti3+ have been theoretically investigated using DFT with PBE exchange and correlation functional. It is found that the most stable B6Ti3+ 01 cluster can maximally adsorb ten hydrogen molecules, which corresponds to a gravimetric uptake capacity of 8.82 wt%. The uptake capacity exceeds the 2015 target set by US Department of Energy for vehicular application. Moreover, the HOMO-LUMO gap value of B6Ti3+ 01 (10H(2)) is larger than that of B6Ti3+ 01, which manifests the B6Ti3+ 01 will be more stable after 10H(2) adsorbed. The hydrogen adsorption energies with Gibbs free energy correction are carried out to reveal whether adsorption of hydrogen on B6Ti3+ is favorable or not at different temperatures. The results indicate that the adsorption of ten hydrogen molecules on B6Ti3+ 01 is energetically favorable in a fairly wide temperature range. Therefore, B6Ti3+ 01 is considered to be a promising material for hydrogen storage. (C) 2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.