Hydrothermal reactions of Na-2[Mo(2)O(4)EDTA](.)5H(2)O and LnCl(3)(.)6H(2)O produce the chiral layered lanthanide molybdate oxides pillared by the chiral cluster ligand, [Ln(H2O)MoO4](2)[lambda-Mo(2)O(4)EDTA] (Ln = Gd, 1; Eu, 2; Tb, 3; Y, 4). The tetradentate molybdate bridges Ln(3+) to form a square grid structure, which is pillared by the chiral cluster ligand, [lambda-Mo(2)O(4)EDTA](2-), into a 3-D chiral framework structure. Strong VCD (vibrational circular dichroism) signals confirm the chirality of the bulk oxide materials. These bimetallic oxide materials are of highly thermal stability. The magnetic interactions between the Ln(3+) ions in 1 and 3 are weak antiferromagnetic.