In recent years, two-dimensional molybdenum disulfide (MoS2) has attracted extensive attention in the application field of next-generation electronics. Compared with single-layer MoS2, bilayer MoS2 has higher carrier mobility and has more promising applications for future novel electronic devices. Nevertheless, the large-scale low-cost synthesis of high-quality bilayer MoS2 still has much room for exploration, requiring further research. In this study, bilayer MoS2 crystals grown on soda-lime glass substrate by sodium chloride (NaCl)-assisted chemical vapor deposition (CVD) were reported, the growth mechanism of NaCl in CVD of bilayer MoS2 was analyzed, and the effects of molybdenum trioxide (Mo) mass and growth pressure on the growth of bilayer MoS2 under the assistance of NaCl were further explored. Through characterization with an optical microscope, atomic force microscopy and Raman analyzer, the domain size of bilayer MoS2 prepared by NaCl-assisted CVD was shown to reach 214 μm, which is a 4.2X improvement of the domain size of bilayer MoS2 prepared without NaCl-assisted CVD. Moreover, the bilayer structure accounted for about 85%, which is a 2.1X improvement of bilayer MoS2 prepared without NaCl-assisted CVD. This study provides a meaningful method for the growth of high-quality bilayer MoS2, and promotes the large-scale and low-cost applications of CVD MoS2.