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This study reports the growth of aligned monolayer molybdenum disulfide (MoS2) ribbons on a sapphire substrate viaNaOH-assisted chemical vapor deposition. The length of MoS2ribbon is up to 400 μm. The MoS2ribbon has excellent single crystal properties, a carrier mobility of {150 cm2V−1s−1, and a optical response of 103 mA W−1at a wavelength of 550 nm. The growth model of MoS2ribbons was given. NaOH reacts with MoO3to form sodium molybdate droplets, which increase the fluidity of the molybdenum source on the substrate, realizing the vapor–liquid–solid growth of MoS2on sapphire. The monolayer MoS2ribbons have two kinds of arrangements on the sapphire substrate, one is the oriented growth affected by the interlayer van der Waals force and the lattice, and the other is the aligned growth constrained by the sapphire step. Our results promote the basic research and device applications of MoS2, and introduce a new way of synthesizing other one dimensional (1D) and 2D nanostructures.