We have calculated the high-symmetry stackings of BL MoS2 to have reference values for our tBL considerations and validation of the employed methods. Figure shows the different BL stacking configurations of MoS2. The lowest-energy 𝐻 ℎ ℎ configuration (Figure ) corresponds to the equilibrium 2H bulk, while the slightly less stable 𝑅 ℎ 𝑀 stacking (Figure ) is also known from the bulk in the 3R form. In both cases, the sulfur atoms in the top layer are eclipsed with the molybdenum atoms in the bottom layer and the interlayer distance is 6.03 Å. Shifting the low-energy stackings to another high-symmetry position, where the sulfur atoms are eclipsed, yields 𝐻 ℎ 𝑀 (Figure ) and 𝑅 ℎ ℎ (Figure ) stackings. The latter one is the perfectly eclipsed configuration. In both cases, the interlayer distance is increased by nearly 0.5 Å and the interlayer interaction is lowered by more than 50 meV per unit cell (uc). A further low-energy stacking, shown in Figure , only slightly (2 meV/uc) higher in energy than the low-energy stackings, is 𝐻 ℎ 𝑋 , which emerges from the lowestenergy configuration and has eclipsed molybdenum atoms. The twist angle 𝜃 is historically defined with respect to both sheets being parallel, which refers to the 𝑅 family of stackings (Figure ). The lowest configuration in this family is metastable 𝑅 ℎ 𝑀 stacking. The lowestenergy 𝐻 ℎ ℎ BL configuration can only be reached by symmetry operations applied to one of the layers, either rotation by 60°, mirroring in a lateral plane, or inversion. Thus, twist angles 𝜃 → 0° will converge to metastable 𝑅 ℎ 𝑀 , while 𝜃 → 60° to lowest-energy 𝐻 ℎ ℎ BL stacking. In Table , all characteristic values for understanding the interlayer interaction energy E IL = 2E ML -E BL and interlayer distance for the five high-symmetry stackings are given for the range of methods employed in this work. Note that, while the interlayer energy differs between various methods, the energy difference between the different stacking types, which is most relevant for this work, agrees. The same holds for the interlayer distance. It is found that the energy differences between the 𝐻 ℎ ℎ and the 𝐻 ℎ 𝑋 stackings are underestimated by ReaxFF. From this, it can be expected that ReaxFF also underestimated the size changes between the non-equivalent stacking domains for twist angles close to 60°.