The title compound Cs [(VO)(2)(OH)(O3PCH2CH2PO3)] 1 was synthesized hydrothermally from a mixture of CsVO3, H2O3PCH2CH2PO3H2, and H2O in the mole ratio 1:1.22:535 and heated to 200 degrees C for 48 hr. Phosphonate 1 is formed in 45% yield and crystallizes in the monoclinic space group P2(1)/c with a=11.798(2) Angstrom, b=11.056(2) Angstrom, c=8.682(2) Angstrom, beta=104.92(3)degrees, V=1094.3(4) Angstrom(3), Z=4, and R=0.054. The framework consists of complimentary inorganic V/P/O layers joined by ethylenediphosphonate ligands, creating an inorganic bilayer, The bilayers are seperated by an interlamellar region of Cs+ cations, There are two unique VO5 square pyramids from which the inorganic V/P/O layers are constructed. (C) 1997 Academic Press.