An imidazole encapsulating indium phosphate with an In:P ratio of 4:7 and a new pillared layer structure has been synthesized under solvothermal conditions and characterized by single-crystal X-ray diffraction, P-31 CPMAS NMR, and thermogravimetric analysis. [Crystal data: [In-8(HPO4)(14)(H2O)(6)](H2O)(5)(H3O)(C3N2H5)(3), M(r) = 2686.72, trigonal, space group P-3c1 (No. 165), a = 13.859(2) Angstrom, c = 19.186(8) Angstrom, V = 3193(4) Angstrom(3), Z = 2, R = 3.6%, R(w) = 3.7% (1650 observed data with I > 3 sigma(I))]. The structure consists of layers assembled from InO6 and InO5(OH2) octahedra and PO3(OH) tetrahedra which are pillared through additional InO6 octahedra to produce a three-dimensional framework. The framework contains a two-dimensional array of channels in which imidazolium cations, hydroxonium ions, and water molecules reside. Within the channels are 16-membered rings of alternating In and P polyhedra which have dimensions similar to 8.6 x 9.7 Angstrom.