An unhydrated phase of the potassium intercalate of the hydrated vanadium oxides in Part 1 has been synthesized in a hydrothermal VO(OH)2aKCl system. It, is formulated as &.5v205 and adopts the monoclinic system C2/m with a= 11.688(2) A, 6 =3.668(1) A, c = 9.505(2) A and = 92.24(1)". A single-crystal structure analysis revealed a 6-Ago.,V205 type structure (R/R, = 0.061 /0.048), which involved a three-dimensional structure of the double-sheet V,05 layer proposed in Part 1. &, 5v205 was converted into a hydrated phase, Ko,V205*H20, by oxidation or by lowering the potassium content, which expanded the layer spacing from 9.50 A to 10.88 A. The reverse change from &.3v205* H20 to &, 5v205 was effected by using a reducing agent such as a potassium iodide solution. The hydration process seems to be controlled by the interlayer potassium content.