Bare titanium dioxides (TiO2) and doped with metal (Cu) or non-metal ion (F) were synthesized by a single-step flame spray pyrolysis (FSP) method. According to the BET, XRD, and TEM results, the Cu-and F-doped TiO2 nanoparticles synthesized by FSP possess comparable features in terms of surface area, crystallite size and phase composition, and morphology. However, the F-doped TiO2 exhibited the highest photocatalytic activity for the complete oxidation of acetaldehyde (ACE) even surpassing benchmarking Aeroxide TiO2 (P25). In contrast, Cu-doped TiO2 had a detrimental effect on the ACE photocatalytic oxidation. The proportion of native terminal hydroxyl groups, evaluated using high-field H-1 MAS NMR, on the particle surface was varied by doping the TiO2 with either Cu or F ions during FSP synthesis. A relationship, whereby decreased terminal hydroxyl group content corresponded to elevated acetaldehyde photodegradation, was subsequently uncovered. The findings were reinforced by studying the XPS O is photopeaks in the region attributed to surface hydroxyl groups. (C) 2012 Elsevier B.V. All rights reserved.