Reducing the dimensionality of inorganic lattices allows for the creation of new materials that have unique optoelectronic properties. We demonstrate that a layered metal chalcogenide lattice, TiS2, can form a dimensionally reduced crystalline one-dimensional hybrid organic/inorganic TiS2(ethylenediamine) framework when synthesized from molecular precursors in solution. This solid has strong absorption above 1.70 eV and pronounced emission in the near-IR regime. The energy dependence of the absorption, the near-IR photoluminescence, and electronic band structure calculations confirm that TiS2(ethylenediamine) has a direct band gap.