Two novel organic amine templated lanthanide sulfates, layer (H(3)DETA)[Nd(H2O)(SO4)(3)] (I) and chain-like (H(3)DETA)[Ho(H2O)(2)(SO4)(3)] (II), are hydrothermally synthesized by using diethylenetriamine (DETA) as template, and are structurally characterized by ICP, elemental analysis, X-ray single-crystal diffraction, X-ray powder diffraction, IR, and TG. Compound I is monoclinic with space group P2(1) and data of unit cell: a = 6.6518(13), b = 10.373(2), c = 11.091(2) , beta = 93.61(3)A degrees, V = 763.7(3) (3), rho (c) = 2.421 g/cm(3), mu(MoK (alpha)) = 3.885 mm(-1), Z = 2, R (1) = 0.0194 for 3312 reflections with F (o) > 2 sigma(F (o)). The Nd ions are nine-coordinated by one oxygen atom of coordinated water and eight oxygen atoms of sulfates. Compound I displays the layer structure constructed by linking Nd ions with three-linkage SO4 tetrahedra as the bridge (affording one coordinated vertex and coordinated edge). Compound II crystallizes in the monoclinic space group P2(1)/c with unit cell data: a = 6.594(13) , b = 14.783(3) , c = 16.599(3) , beta = 93.47(3)A degrees, V = 1614.2(6) (3), rho (c) = 2.454 g/cm(3), mu(MoK (alpha)) = 5.37 mm(-1), Z = 4, R (1) = 0.0259 for 1815 reflections with F (o) > 2 sigma(F (o)). The Ho ions are eight-coordinated by two oxygen atoms of coordinated water and six oxygen atoms of sulfates. The straight chain-like structure of II is attained by alternatively arranging HoO8 polyhedra and two-linkage SO4 tetrahedra (affording two coordinated vertices). The TG results indicate that the two compounds experience three weight losses and lead to distinct residues: Nd2O3 for I and HoO(SO4)(0.5) for II.