High-energy, inexpensive and safe electrochemistries have been the main goals of lithium-ion battery research for many years. Historically, manganese-based cathodes have long been studied for their attractive cost and safety characteristics [1]. However, due to issues related to both surface and bulk instabilities, manganese-rich electrodes have yet to find substantial success in the high-energy lithium-ion battery market. With current trends in cathode chemistries leaning heavily toward Ni-rich compositions, the factors of cost and safety are again at the forefront of research and development efforts. This paper reports the recent progress made at Argonne National Laboratory (USA) to stabilize manganese-rich cathode structures and surfaces with a specific focus on composite materials with intergrown layered and spinel components; it presents an overview of their electrochemical properties in terms of capacity, energy, and cycle-life in cells with metallic lithium, graphite, and Li4Ti5O12 anodes. These layered-spinel cathodes show promise as alternatives to highly nickel-rich electrode compositions, which bodes well for continued advances.