A series of isomorphic lanthanide metal-organic frameworks (Ln-MOFs), {[Ln(L)(H2O)(2)]center dot 5H(2)O} (1-Ln, where Ln = Eu, Tb, Gd, and EuxTb(1-x)), have been synthesized by a rigid 1,3-bis(3,5-dicarboxyphenyl)imidazolium chloride (H4L+Cl-) ligand and Ln(3+) ions via a solvothermal method. Single-crystal X-ray diffraction indicated that 1-Ln exhibited similar three-dimensional porous frameworks with one-dimensional channels decorated by the uncoordinated carboxylate oxygen atoms. The luminescent sensing studies indicated that 1-Eu is an outstanding reusable luminescent probe suitable for the simultaneous detection of Cr2O72-, CrO42-, and MnO4- ions in an aqueous solution. Remarkably, the different proportions of Eu3+ and Tb3+ can be combined into the same Ln-MOF to yield a new series of differently doped 1-EuxTb1-x MOFs. At the same excitation wavelength, they generated dual-emission peaks of Eu3+ and Tb3+ to show a gradual change in luminous color between yellow-green, yellow, orange, orange-red, and red. On the basis of the excellent optical properties of 1-Ln complexes, they can be employed as promising luminescent probe and multicolor tunable photoluminescence materials.