We report on the preparation and electrochemical characterization of Li 2 M(SO 4) 2 (M=Co, Fe), where the Fe-based phase was previously unknown. Both compounds can be made at low temperatures (b 320 °C) and the Fe-based phase displays an open circuit voltage of 3.83 V vs. Li + /Li 0 for the Fe 3+ /Fe 2+ redox potential. This corresponds to the highest voltage ever obtained for the Fe 3+ /Fe 2+ redox couple in an iron-based, fluorine-free compound and is only matched by the triplite phase of LiFeSO 4 F. While the theoretical capacity of 102 mA h g − 1 will likely limit the commercial prospects for this phase, knowledge of the structure will provide useful insight into the structural origin of these increased potentials.