The layered LiCoO2 compound, which has been of great interest for lithium-ion batteries, was prepared in this paper by calcining an ethylenediaminetetraacetic acid (EDTA)-based complex precursor crystal at low temperatures. The details of the synthesis procedure are presented and a possible mechanism of formation for the EDTA/Co/Li complex precursor is discussed. The physical properties of the synthesized cathode materials are discussed in the light of structural (X-ray diffraction! and thermal (differential thermal! analyses. The charge and discharge cycling characteristics of cells containing the synthesized LiCoO2 as positive electrode and lithium metals as anode with a nonaqueous electrolyte showed that the LiCoO2 synthesized at 700degreesC exhibited much better performance than the materials obtained by conventional solid-state reaction techniques with a first cycle capacity of 167 mAh/g and specific capacity loss of about 11% for 30 cycles.