Despite the fact that new dimensionally reduced hybrid organic inorganic compounds have attracted considerable interest because of their unique optical and electronic properties, the rational synthesis of these new materials remains elusive. Here we systematically studied the relative influence of the major synthetic parameters, including temperature, ligand structure, and ligand-to-metal stoichiometry, on the preparation of dimensionally reduced TiS2. One-dimensional TiS2 phases tend to form at high ligand-to-metal ratios and relatively lower temperatures, while the two-dimensional parent lattices are preferred at higher temperatures. The organic ligand structure dictates the temperature window in which a dimensionally reduced phase can be accessed. Although a small change in ligand structure, such as changing ethylenediamine to propylenediamine, for example, will significantly influence the stability of these phases, it will only subtly change the electronic structure. Via the development of a systematic understanding of the effects of various factors during the synthesis, this work provides a pathway to rationally create new dimensionally reduced materials.