Two-dimensional (2D) single sheets formed via delamination of Layered Double Hydroxides (LDHs) are of great interest because of their high reactive surface area and unique chemical and physical properties. Here, we focus on formation and properties of single sheet iron oxides (SSI) that may be used as sorbents, electro-and photocatalysts. We have developed a method for synthesis of SSIs from the Fe II -Fe III LDH (green rust, GR) using surfactant intercalation of preformed GR, followed by aerial oxidation and delamination. The average height of the SSIs from AFM is 1 nm and the lateral dimensions vary from 20 to 100 nm. Selected area electron diffraction of SSI shows a hexagonal pattern with d ≈ 0.28 nm consistent with diffraction along [001] in metal hydroxide layers in GR. Chemical analysis, thermogravimetric analysis and X-ray photoelectron spectra analysis lead to SSI formula of FeO 0.82 (OH) 1.38 • 0.7H 2 O. For the oxidized, surfactantintercalated GR and SSI, pair distribution functions from high energy X-ray scattering data demonstrate that two distinct interatomic distances exist for first neighbor Fe-Fe pairs, somewhat similar to the patterns for ferrihydrite and goethite, but in contrast to the single Fe-Fe distance observed for the unoxidized GR. A modeled structural rearrangement with vertical displacements of Fe atoms from the original hydroxide layer to form a trilayer with Fe polyhedra that are linked via both corner-and edge-sharing produced a PDF in agreement with the main features of the measured pattern. Mössbauer spectroscopy shows that the SSI orders magnetically at 130 K and that the hyperfine parameters are distinct for SSI and different from other iron oxides such as ferrihydrite and feroxyhite. The synthesis pathway via GR C12 is critical for formation of SSI as the "insolating" C12 interlayer hinders bonding and polymerization between Fe III -O/OH octahedra across interlayers during oxidation and thus only structural reorganisations of single brucitic Fe II -Fe III hydroxide layers can take place during oxidation with no possibilities for nucleation of iron oxides with higher crystallinity like goethite. The strong increase of single-and double coordinated O/OH groups in the SSI compared with the parent GRs predicts a high reactivity of SSI as surface complexation sorbents.