This synthesis procedure has been extended to the one-pot synthesis of nano-alumina based Ag catalysts with spherical and rod-shaped nano-alumina morphologies. Selective catalytic reduction (SCR) of NO with C3H6 over these catalysts was investigated. The results were compared to those of the conventional Ag/γ-Al2O3 and γ-nanoalumina alone. These nano-alumina based Ag catalysts exhibit excellent NO reduction activity in the presence of C3H6. Even in the presence of large oxygen concentration (15%), N2 yields as high as ∼90% at quite low temperature (∼350 °C) have been achieved. The significantly high catalytic activity of this new type of nanocatalysts can also be attributed to their high surface area and good dispersion of silver species in the alumina matrix as well as the synergism and new properties that arise at the silver-nanoalumina interface.