The hydrothermal synthesis, crystal structure analysis, and spectroscopic studies of InPO4·2H2O (1) and InAsO4·2H2O (2) are reported. Compound 1 is isomorphic with metavariscite: monoclinic P21/n (No. 14), a = 5.4551(3) Å, b = 10.2293(4) Å, c = 8.8861(3) Å, β = 91.489(4)°, Z = 4, and compound 2 is isomorphic with variscite: orthorhombic Pbca (No. 61), a = 10.478(1) Å, b = 9.0998(8) Å, c = 10.345(1) Å, Z = 8. Their three-dimensional frameworks are built of corner sharing InO4(H2O)2 octahedra and MO4 (M = P5+ or As5+) tetrahedra. The water molecules in both compounds have different environments and are involved in different types of hydrogen bonding. Infrared spectroscopy indicates that water molecules are true H2O species.