Next generation batteries needed for numerous consumer and vehicular applications require improved electrochemical charge storage materials that have higher capacities, improved rate capabilities, and longer cycle lives.  Nanosheets consisting of atomic two-dimensional (2D) layers have a number of key features for cathodes including rapid surface-based charge storage rather than intercalation, quantum confinement in two dimensions, and the ability to accommodate substantial structural changes during insertion/de-insertion.  We have explored transition metal (M=V, Fe, Mn) oxide nanosheets to provide improved cathodes for Li-ion and Mg-ion batteries.  Synthesis conditions were controlled to obtain nanosheets with controlled sheet sizes, phase, and aggregation.  Temperature treatments were found to significantly affect the electrochemical charge and discharge capacities with in some cases lower temperature treatments providing improved performance over higher temperature treatments.   Using different drying conditions was explored as a route to maintain largely distinct nanosheets and prevent nanosheet restacking which facilitates the storage of larger cations (e.g. Mg-ions).  Obtaining oriented nanosheets through using substrate interactions and applied fields was investigated to increase the electronic conductivity and improve the rate capabilities.   The ability to control the structure and properties of transition metal oxide nanosheets provides a route to cathodes with improved capacities, rates and cycle life.