Using P-31 and C-13 NMR with DFT calculations we demonstrate the exposed surface of titania nanotubes (TiNTs) is a stable, unterminated anatase (0 0 1)-like surface and is catalytically active under ambient conditions. We find that methanol dissociatively adsorbs on the surface of TiNTs agreeing with the predicted activity of surface dissociation of organic molecules on the crystalline (0 0 1)-anatase surface. We further examined the catalytic activity of anatase power, TiNT, and nanosheets in catalytic hydrolysis of S-[2-(diisopropylamino)ethyl]-O-ethyl methylphosphonothioate (VX) via P-31 NMR and demonstrate that titanate-like nanosheets are inactive in the reaction owing to their hydroxylated (0 0 1) surface. (C) 2009 Elsevier B.V. All rights reserved.