In their recent Letter, Klein and Zottola [Chem. Phys. Lett. 419 (2006) 254-258] emphasized the superior performance of density functional theory combined with the 6-311 ++G(2d, p) Pople-style basis set relative to conventional methods, such as second order perturbation theory and coupled cluster theory, with correlation consistent basis sets for the prediction of bond lengths. In this work, we present evidence that the former approach may be less capable of achieving uniformly accurate results for a variety of spectroscopic properties. (c) 2006 Elsevier B.V. All rights reserved.