The structures of the hydrated thallium(III) halide and pseudohalide complexes, [TlX(n)(OH2)(m)]((3-n)+), X = Cl, Br, CN, in aqueous solution have been studied by a combination of X-ray absorption fine structure spectroscopy (XAFS), large-angle X-ray scattering (LAXS), and vibrational spectroscopic (Raman and IR) techniques including far-infrared studies of aqueous solutions and some solid phases with known structures. The vibrational Tl-X frequencies of all complexes are reported, force constants are calculated using normal coordinate analysis, and assignments are given. The structural results are consistent with octahedral six-coordination for the cationic complexes Tl(OH2)(6)(3+), TlX(OH2)(5)(2+), and trans-TlX(2)(OH2)(4+). The coordination geometry changes to trigonal bipyramidal for the neutral TlBr3(OH2)(2) complex and possibly also for TlC3(OH2)(2). The TlX(4)(-) complexes are all tetrahedral.