LiCoO2 cathode materials have been prepared by a spray-drying technique. The stoichiometry of the materials, their morphology, and the phase composition and electrochemical performance have been studied. The effects of thermal annealing and decomposition processes on the structure are discussed in detail. The changes of Li content in materials were monitored by ICP spectrometry. It was established that the decomposition of the acetates at around 450°C is a slurry-making process that compacts the powder. It was found that well lithiated samples with good life cycle and high capacity can be prepared using acetate precursors and a spray solution technique. The morphology, grain size and texturing can be controlled by the sintering time and temperature in combination with intermediate grinding.