To extrapolate the electronic band structures to twist angles 𝜃 < 2° and 𝜃 > 58°, the obtained TB parameters as function of the moiré cell's lattice constant were fitted with an exponential function. These were then used to estimate on-site elements and hopping terms and, thus, the electronic band structures for 𝜃 → 0° and 𝜃 → 60°. For the hcb lattices, all tBL MoS2 structures were used, and the extrapolation function was chosen as 𝑦 = 𝐴 1 𝑒 -𝑏 1 /𝑥 + 𝐴 2 𝑒 -𝑏 2 /𝑥 + 𝑦 0 to ensure a good agreement. For the kgm lattices, the 8 structures closest to 0° and 60° were used and the extrapolation function was chosen as 𝑦 = 𝐴𝑒 -𝑏/𝑥 + 𝑦 0 . The offset 𝑦 0 was only included for extrapolating the on-site elements; for the hopping terms it was set to 𝑦 0 = 0.