The concept of asymmetric solvation in I- (CH3CN)(2) clusters [C. E. H. Dessent, C. G. Bailey, and M. A. Johnson, J. Chem. Phys. 103, 2006 (1995)] was revisited in light of quantum chemistry calculations of the cluster structures, energetics and charge-transfer-to-solvent transition energies. In addition to the two "classical" linear structures-with a symmetrically and an asymmetrically solvated iodide-that were postulated previously, a nonlinear hydrogen-bonded isomer was also found. The calculated binding energies and vertical excitation energies for the linear symmetric and nonlinear hydrogen-bonded I- (CH3CN)(2) isomers are in very good agreement with experimental data, while the linear asymmetric structure appears unlikely to be involved in experiments. The importance of hydrogen bonding in halide-acetonitrile clusters manifests itself, not only in the fact that a stable nonlinear hydrogen-bonded isomer exists, but also in slight geometrical distortions of the "classical" linear cluster structures.