Although the synthesis of molybdenum disulfide (MoS₂) on sapphire has made a lot of progress, how the substrate surface affects the growth still needs to be further studied. Herein, the impact of the sapphire step height on the growth of monolayer MoS₂ through chemical vapor deposition (CVD) is studied. The results show that MoS₂ exhibits a highly oriented triangular grain on a low-step (0.44–1.54 nm) substrate but nanoribbons with a consistent orientation on a high-step (1.98–3.30 nm) substrate. Triangular grains exhibit cross-step growth, with one edge parallel to the step edge, while nanoribbons do not cross steps and possess the same orientation as the step. Scanning electron microscopy (SEM) reveals that nanoribbons are formed by splicing multiple grains, and the consistency of the orientation of these grains is demonstrated with a transmission electron microscope (TEM) and second-harmonic generation (SHG). Furthermore, our CP2K calculations, conducted using the generalized gradient approximation and the Perdew–Burke–Ernzerhof (PBE) functional with D3 (BJ) correction, show that MoS₂ domains prefer to nucleate at higher steps, while climbing across a higher step is more difficult. This work not only sheds light on the growth mechanism of monolayer MoS₂ but also promotes its applications in electrical, optical, and energy-related devices.