This paper presents synthesis and electrochemical properties of tetragonal lithium manganese dioxide, Li2Mn2O4 and its cobalt doped analogue Li2Co0.4Mn1.6O4. The materials are compared as host materials for lithium insertion and the behavior during the initial lithium extraction as well as on repeated cycling is presented. These materials show an initial lithium extraction capacity between 200 and 270 mAh/g. On repeated cycling, they are converted into spinel-like lattices with reversible capacities in the range 82–90 mAh/g. As they are chemically compatible with the manganese spinel, they will be well suited as additives compensating for the capacity loss during the initial forming cycle of spinel-based lithium-ion cells.