The structural and electronic properties of the intercalation compound LixTiS2, x = 1/4, 3/4, and 1, are investigated at the ab initio, all-electron, periodic Hartree-Fock level, using an extended basis set and a posteriori density functional correlation corrections to the total energy, Calculated lattice parameters, bulk moduli, linear moduli, cohesive energy, elastic constants, band structure? density of states, and Mulliken populations are reported. This study indicates that the following physical changes in LixTiS2 are induced by intercalation. (1) The crystal expands uniaxially in the (c) over right arrow direction. (2) The S-Ti-S layers expand negligibly (<0.01 Angstrom) in the (c) over right arrow direction at x = 1/4, but a large (0.16 Angstrom) layer expansion occurs at x = 1. (3) The elastic properties change negligibly at x = 1/4, but the interlayer stiffness c(33) increases by a factor of similar to 4 at x = 1. (4) Lithium charge is donated to the S(3p) and Ti(3d) orbitals. At least 75% of this charge is acquired by sulfur atoms. (5) At x = 1/4, the donated charge is localized over the lithium near-neighbor S(3p) and Ti(3d) orbitals. (6) Charge transfer to a Ti(3d)-based conduction band yields metallic properties.