A series of layered-type pseudo four-component Li-Ni-Co-Ti oxides were prepared to explore optimal cathode materials for a lithium-ion secondary battery. The new layered-type compounds were prepared using a combinatorial material-preparation system based on electrostatic spray deposition (the "M-ist Combi'' system), and combinatorial powder X-ray diffraction. The composition region of the new compounds (Li-alpha(NixCoyTiz)O-2 (a similar to 1, 0 <= x <= 1, 0 <= y <= 1, z similar to 0.2, x + y + z = 1.0)) was found to be wider than the composition region previously reported (LiNi0.8-yCo0.2TiyO2 (0 <= y <= 0.1)). (C) 2007 Elsevier B.V. All rights reserved.