Complex Sol-Gel Process (CSGP) was applied to the preparation of LiNi0.5Co0.5O2. Starting sol-solutions were prepared in two different ways: I, in which aqueous ammonia was added to a starting solution of Li+-Ni2+-Co2+ acetate-ascorbate, and II in which LiOH was added to a solution of Ni2+- Co2+ and NH4
+ acetate-ascorbate. It was found that in the absence of ascorbic acid, or at its lower content (≤0.2 M on 1M σ Li+- Ni2+- Co2+) precipitation of Ni hydroxides occurred. Regular sols were concentrated ∼3 times, gelled and dried at 140°C. Intensive foaming was observed for samples during further heating. Consequently for scaling up to 200g in a run a preliminary long drying procedure followed by self-ignition step (∼400°C) was introduced. Thermal transformation of the gel to solid was studied by TG, DTA, XRD and IR. The main feature of this step is carbonate formation. The final structure LiNi0.5Co0.5O2 is observed after heating for Ih at 800°C. For larger scale production the extension of firing time was necessary. Electrochemical properties of the LiNi0.5Co0.5O2 compound, prepared by the CSGP were evaluated and considered satisfactory.