The necessity of developing low-cobalt cathode oxides for lithium-ion batteries is increasingly apparent. The most popular strategy followed thus far in addressing this issue has been the development of LiNiO2-like, Ni-rich, layered LiMO2 (M = Ni, Mn, Co; NMC) oxides with low Mn and Co contents, e.g., NMC-811. However, safety, cycle-life, and even cost could remain critical barriers to the success of such cathode materials. Herein an alternative to LiNiO2-based, low-cobalt cathodes is suggested based on modifications to the prototypical cobalt-free, layered oxide, LiNi0.5Mn0.5O2.