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Energies, structural parameters, and harmonic vibrational frequencies of the linear carbon–sulfur clusters, CnSm (n = 1–29, m = 1–2), have been computed using density functional theory (DFT) with the B3LYP exchange‐correlation functional and Pople's 6‐311G* basis set. The energies and equilibrium geometries have been compared to MP2 (Møller–Plesset second‐order perturbation) and CCSD(T) calculations for C2S, C6S, and C7S2, three carbon–sulfur clusters recently observed and reported for the first time in the following article. The vibrational frequencies, predicted using B3LYP/6‐311G*, agree satisfactorily with the observed infrared (IR) band frequencies, with only a 17 cm−1 standard deviation for all experimentally known carbon–sulfur cluster C—C stretching modes. Dissociation energies calculated for different loss mechanisms indicate that carbon–sulfur clusters prefer to lose CS, in agreement with experimental observations. © 2004 Wiley Periodicals, Inc. Int J Quantum Chem, 2005 [ABSTRACT FROM AUTHOR]