We present a density functional study on the structural and electronic properties of ZnS bubble clusters, specifically, hollow cages whose spontaneous formation was previously observed in classical molecular dynamics simulations by Spano et al. [J. Phys. Chem. B 2003, 107, 10337]. The hollow ZnS cages in our study were modeled as ZnxSx [x = 12, 16, 24, 28, 36, 48, 108], and an onionlike structure was modeled as Zn96S96. The study of energetics and stability, performed using large polarized Gaussian basis sets, indicated all structures to be energetically stable with similar binding energy of 5.5-5.6 eV per ZnS pair. Further computation of electronic properties showed that these cages have large vertical ionization energies and relatively low electron affinities in the ranges of 6.8-8.1 and 1.7-3.0 eV, respectively. They have large highest occupied molecular orbital lowest unoccupied molecular orbital gaps between 2.5 and 3.3 eV, and quasi-particle gaps vary from 6.2 eV for Zn(12)Sto 4.19 for Zn108S108. The computed vibrational frequencies for selected cages, that is, Zn12S12, Zn16S16, Zn28S28 (0, S-4, and S-8 point groups), and Zn36S36 indicate that these cage structures correspond to local minima on the potential energy surface. Finally, the infrared spectra calculated using large basis sets are also reported.