We investigated the initial growth of ${\mathrm{TiTe}}_2$ on Au(111) from submonolayer to multilayer coverage by scanning tunneling microscopy (STM), low-energy electron diffraction intensity analysis (LEED-IV), and density functional theory. In the submonolayer regime, we find a stable and well-ordered ${(5\times \sqrt{3})}_{\mathrm{rect}}$ superstructure consisting of separated ${\mathrm{TiTe}}_2$ molecules, whereby the Ti atoms substitute Au atoms of the first substrate layer as proven by LEED-IV. By adding further Ti and Te in a 1:2 ratio and proper annealing dealloying sets in and a homogeneous $1T-{\mathrm{TiTe}}_2$ monolayer film on an unreconstructed substrate is formed. The resulting moiré structure is close to a $(4\times 4)$ superstructure with respect to Au(111) and has a slightly expanded in-plane lattice parameter compared to the $1T-{\mathrm{TiTe}}_2$ bulk value. With further stoichiometric deposition, thicker $1T-{\mathrm{TiTe}}_2$ films grow. Surprisingly, a five-layer thick film exhibits an even larger lattice parameter ($1.5\%$ larger than the bulk value). All LEED-IV analyses are based on best-fit $R$ factors of $R\le 0.13$.

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• Multilayer thin films
• Thin films
• Transition metal dichalcogenides
• Current-voltage low-energy electron diffraction
• Density functional theory
• Low-energy electron diffraction
• Scanning tunneling microscopy