CeO 2 nanoparticle-decorated α-MnO 2 nanotubes (NTs) were prepared and tested for elemental mercury (Hg 0 ) vapor removal in simulated natural gas mixtures at ambient conditions. The composition which had the largest surface area and a relative Ce/Mn atomic weight ratio of around 35% exhibited a maximum Hg 0 uptake capacity exceeding 20 mg•g −1 (2 wt %), as determined from measurements of mercury breakthrough which corresponded to 99.5% Hg 0 removal efficiency over 96 h of exposure. This represents a significant improvement in the activity of pure metal oxides. Most importantly, the composite nanosorbent was repeatedly regenerated at 350 °C and retained the 0.5% Hg 0 breakthrough threshold. It was projected to be able to sustain 20 regeneration cycles, with the presence of acid gases, CO 2 , and H 2 S, not affecting its performance. This result is particularly important, considering that pure CeO 2 manifests rather poor activity for Hg 0 removal at ambient conditions, and hence, a synergistic effect in the composite nanomaterial was observed. This possibly results from the addition of facile oxygen vacancy formation at α-MnO 2 NTs and the increased amount of surface-adsorbed oxygen species.