Information about the elementary processes involved in heterogeneous catalysis is often obtained from studies with well-defined crystal surfaces. However, current techniques are not efficient in preparing the desired well-defined crystal surfaces. In particular, preparation of MgO (111) has remained illusive to date although theoretical studies have predicted its' stability in the form of a hydroxide. Recently, we reported a simple, efficient and cheap wet chemical route for preparation of MgO (111) nanosheets. We have discovered that MgO nanosheets possessing the exposed (111) plane as a main surface can grow preferentially from magnesium methoxide-benzyl alcohol via self-assembly through slow hydrolysis. The MgO (111) nanosheets have a thickness of less than 10 nm, typically between 3 and 5 nm. The (111) surface is particularly interesting; because it possesses alternating polar monolayers of negatively charged oxygen anions and positively charged magnesium cations. Thus, a strong electrostatic field perpendicular to the (111) surface is created. Such a surface has provided a prototype for the study of surface structure and surface reactions of oxides, which drew great attention for both experimental and theoretical studies. The MgO (111) nanosheets have been studied by in-situ DRIFT spectroscopy and TPD revealing insights into the surface chemistry. Additionally, the catalytic properties of the nanosheets for the Claisen-Schmidt reaction and low temperature decomposition of methanol have been studied and mechanistic insights have been elucidated spectroscopically.