The controlled production of two-dimensional atomically thin transition metal dichalcogenides (TMDs) is fundamentally important for their device applications. However, the synthesis of large-area and high-quality TMD monolayers remains a challenge due to the lack of sufficient understanding of growth mechanisms, especially for the chemical vapor deposition (CVD). Here we report molten-salt assisted CVD growth of highly crystalline MoSe2 monolayers via a novel vapor-liquid-solid (VLS) mechanism. Our results show that the growth rate of the VLS-grown monolayer MoSe2 is about 40 times faster than that of MoSe2 grown via the vapor-solid (VS) mechanism, which makes the fabrication of 100 μm domains for ∼2 min and a uniform monolayer film within 5 min. The ultrafast growth of monolayer MoSe2 crystals benefits from the synergic effect of one-dimensional VLS growth and two-dimensional VS edge expansion. Moreover, these MoSe2 monolayers exhibit high crystal quality and enhanced photoluminescence due to efficient Se-vacancy repairing by the doping of halogen atoms. These findings provide a new understanding of MoSe2 growth and open up an opportunity for the rapid synthesis of high-quality TMD monolayers and heterostructures.