We present a layered Li-intercalation oxide that operates on the V3+/V4+ redox couple. The stabilization effect of adding a +3 element into the layered LiVO2 has been studied by first principles calculations. We identified Cr substitution into LiVO2 to be promising for stabilizing a layered material based on the V redox couple. Layered LiCrxV1-xO2 (x = 0.1, 0.2, 0.4, 0.5) has been synthesized and tested electrochemically. The improved capacity retention confirms that the structural stability of delithiated LiVO2 is improved by Cr doping.