Weakly bound 1: 1 complexes formed between CS2 and a dihalogen molecule XY = Cl-2, Br-2, BrCl, ICl, or IBr have each been trapped in an Ar matrix and hence investigated experimentally by their IR spectra as well as theoretically by MP2 and density functional calculations. A planar structure, with an intermolecular angle close to 90, is expected for such a S=C=S center dot center dot center dot XY molecular complex. Moreover, for each system involving a heteronuclear dihalogen, two possible complexes exist, viz., S=C=S center dot center dot center dot XY and S=C=S center dot center dot center dot YX. The calculated structures, vibrational properties, and binding energetics of the complexes are analyzed, and the NBO formalism is used to interpret their bonding properties. The IR spectra of the complexes thus simulated provided vital guidance for the interpretation of the matrix spectra. For example, complexation was predicted and observed (i) to induce red shifts of the principal absorptions associated with both the CS2 and XY components and (ii) to result, through the change in symmetry, in activation of some modes that are IR-silent for the free components.