In this work, an atomic layer deposition approach for the synthesis of MoS2 monolayers is presented. Optical properties of the prepared large-area samples were characterized by Raman and photoluminescence (PL) spectroscopies, yielding homogeneous optical properties in 5 × 5 mm2 areas. High-resolution transmission electron microscopy and atomic force microscopy demonstrate closed films with grain sizes in the micrometer range. Crucial process parameters and their impact on the properties of the resulting layers are discussed, highlighting the resilience of the process with a broad parameter window for obtaining monolayer films with a high PL yield.