Seven compositions of LiMO 2 (M=LiwNixCoyMnz) (w=1/15−1/6; x=0−3/10; y=1/5−1/2; z=13/30−1/3; i.e. w+x+y+z=1) solid solutions were synthesized using the sol–gel method with the following end members LiCoO 2 , Li 2 MnO 3 (Li[Li 1/3 Mn 2/3 ]O 2 ), and Li[Ni 0.5 Mn 0.5 ]O 2 . The electrochemical behavior of the solid solutions was analyzed for the various compositions of metals in transition metal sites. All synthesized particles were semi-spherically shaped with a layered structure. When the content of lithium and cobalt was reduced (while the other metals were increased), the lattice parameters, a and c, decreased and were accompanied by a shift in the Raman spectrum. The cycling studies reveal that the compound, Li[Li 1/12 Ni 1/4 Co 1/4 Mn 5/12 ]O 2 was found to be optimal in voltage and from a stability point of view.