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Two-dimensional (2D) nanomaterials have distinct optical and electrical properties owing to their unique structures. In this study, smooth 2D amorphous tin disulfide (SnS 2 ) films were fabricated by atomic layer deposition (ALD), and applied for the first time to photoelectrochemical water splitting. The optimal stable photocurrent density of the 50-nm-thick amorphous SnS 2 film fabricated at 140 °C was 51.5 µA/cm 2 at an oxygen evolution reaction (0.8 V vs. saturated calomel electrode (SCE)). This value is better than those of most polycrystalline SnS 2 films reported in recent years. These results are attributed mainly to adjustable optical band gap in the range of 2.80 to 2.52 eV, precise control of the film thickness at the nanoscale, and the close contact between the prepared SnS 2 film and substrate. Subsequently, the photoelectron separation mechanisms of the amorphous, monocrystalline, and polycrystalline SnS 2 films are discussed. Considering above advantages, the ALD amorphous SnS 2 film can be designed and fabricated according to the application requirements.