Abstract Most chemical vapor deposition methods for transition metal dichalcogenides use an extremely small amount of precursor to render large single-crystal flakes, which usually causes low coverage of the materials on the substrate. In this study, a self-capping vapor-liquid-solid reaction is proposed to fabricate large-grain, continuous MoS 2 films. An intermediate liquid phase-Na 2 Mo 2 O 7 is formed through a eutectic reaction of MoO 3 and NaF, followed by being sulfurized into MoS 2 . The as-formed MoS 2 seeds function as a capping layer that reduces the nucleation density and promotes lateral growth. By tuning the driving force of the reaction, large mono/bilayer (1.1 mm/200 μm) flakes or full-coverage films (with a record-high average grain size of 450 μm) can be grown on centimeter-scale substrates. The field-effect transistors fabricated from the full-coverage films show high mobility (33 and 49 cm 2 V −1 s −1 for the mono and bilayer regions) and on/off ratio (1 ~ 5 × 10 8 ) across a 1.5 cm × 1.5 cm region.