A unique composite cathode structure for Li-ion batteries, designated LT-LiNi_1/3Mn_1/3Co_1/3O₂ (or LT-NMC111), has been prepared by flame spray pyrolysis and subsequent annealing between 400 and 650 °C. It is composed predominantly of structurally-integrated and partially-disordered lithiated-spinel and layered components, both of which can be broadly described as partially-disordered rock salt constituents. The paper describes the evolution of the LT-NMC111 structure as a function of the synthesis method, annealing temperature, and electrochemical properties in the context of other recently reported “low-temperature” (LT) materials, such as LT-LiCo_1−xAl_xO₂ and LT-LiMn_0.5Ni_0.5O₂ or, in spinel notation, LT-Li₂Co_2–2xAl_2xO₄ and LT-Li₂MnNiO₄, respectively.