Homogeneously distributed TiO2 nanoparticles with (001) reactive facets were grown over nitrogen-doped reduced graphene oxide sheets (N-rGO) under solvothermal conditions. Hydrogen storage capacity of the system was significantly improved to 0.91 wt% at room temperature and pressure of 0.8 MPa that is the highest hydrogen storage ever reported for graphene-based nanocomposites at room temperature and low pressures. Importantly, this nanocomposite exhibits similar to 91% capacity retention through 5 cycles with more than 88% release of the stored hydrogen at ambient conditions. Enhanced hydrogen uptake and capacity retention were attributed to the synergistic effect of i) reactive facets of TiO2, ii) high dispersion of nanoparticles with the average size of 6 rim, and strong interaction between substrate and TiO2 nanoparticles through polarized C-N bonding of N-rGO sheets. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.