We present a novel method for synthesizing oxidation-free MoS2 films, focusing on interface mechanisms. By utilizing a sulfurization-free solution process and single-step annealing, we fabricate films on Si3N4 surfaces with improved uniformity, exhibiting surface roughness below 0.5 nm and a 4 nm thickness at a precursor concentration of 30 mM, annealed between 700 and 800ºC. Characterization reveals a hexagonal lattice structure with crystallographic orientations of (1 1 0 0) and (1 2 1 0), featuring lattice spacings of 0.27 nm and 0.16 nm, respectively. XPS analysis on SiO2 substrates shows migration of oxygen species, evidenced by a Si 2p spectrum shift to binding energies between 102.6 eV and 102.8 eV. MoS2 films on Si3N4 exhibit a complex Si 2p peak evolution between 100.9 eV and 101.8 eV, providing insights into oxide-free MoS2 film synthesis for advanced electronic devices. This dataset includes all the raw data associated with this study.