Chemical deintercalation of lithium ions was attempted on Li2MoO3 with a structure related to the α-NaFeO2 type structure. The lithium ions in Li2-xMoO3 were removed up to x=0.77 by oxidation, and its structure remained almost unchanged. The evolution of the lattice parameters for deintercalation compounds was divided into two parts; the regions of 01/3Mo2/3)O2)n layer to the interlayer spaces. Magnetic properties of Li2-xMoO3 exhibited temperature-independent paramagnetism.