The indium(I) complex [Tp(But2)]In([Tp(But2)] = tris(3,5-di-tert-butylpyrazolyl)hydroborato), synthesized by the reaction of [Tp(But2)]Na with InCl, exhibits a structure in which the [Tp(But2)] ligand adopts a highly twisted configuration due to steric interactions of the tert-butyl substituents in the 5-positions of the pyrazolyl groups. In contrast, the absence of 5-tert-butyl substituents allows the pyrazolyl groups in [Tp(But)]In to be coplanar with their respective In-N-N-B planes. The structure of [Tp(But)]In has been previously reported but was noted to exhibit an unusual type of disorder in which a nitrogen atom of one molecule was coincident with the boron atom of its disordered configuration [Dias, H. V. R.; Huai, L.; Jin, W.; Bott, S. G. Inorg. Chem. 1995, 34, 1973-1974]. In view of the unusual nature of the disorder, which involved both a 2-fold rotation and a canting of the molecule, the disordered structure of [Tp(But)]In was re-evaluated. Significantly, an ordered structure of [Tp(But)]In was obtained. The disorder present in the previously reported structure is a consequence of adopting a space group with unnecessarily high symmetry. Thus, [Tp(But)]In provides an example where the structure is much better described as ordered in a noncentrosymmetric space group, rather than disordered in the centrosymmetric alternative. [Tp(But)]In is monoclinic, of space group P2(1)/c (No. 14), with a = 18.781(9) Angstrom, b = 10.380(2) Angstrom, c = 20.849(6) Angstrom, beta = 112.76(3)degrees, and Z = 4. [Tp(But)]In is orthorhombic, of space group Cmc2(1) (No. 36), with a 16.193(3) Angstrom, b = 15.214(3) Angstrom, c = 9.963(3) Angstrom, and Z = 4.