Twisted bilayers of MoS2 were constructed by placing two MoS2 monolayers on top of one another with an interlayer distance of 6.3 Å between the planes of the Mo atoms and introducing a twist angle, 𝜃. Structures with 𝜃 → 0° (𝜃 → 60°) were created starting from BLs with 𝑅 ℎ 𝑀 (𝐻 ℎ ℎ ) stacking, where the sulfur atoms of the top layer are placed eclipsed to the molybdenum atoms of the bottom layer. The individual layers were then rotated relative to each other by a twist angle between 2° (58°) and 6.01° (53.99°). The 𝜃 values were chosen so that finite unit cells with commensurate layers and no isotropic strain were obtained. This resulted in a total of 24 structures. For example, the unit cells for 𝜃 = 2° and 𝜃 = 58° contain 4902 atoms and have a moiré lattice constant of 91 Å .