The size of the moiré cell as function of the twist angle is given in Figure . The structures at 2° and 58° have the largest moiré cells for which we can solve the electronic system explicitly using DFTB. To extrapolate to even larger moiré cells, we fitted the calculated bands to a TB Hamiltonian with symmetry-adopted hopping elements as outlined in Figure ). Here, we describe the bands of the hcb and the kgm lattices independently from each other. The fitted TB parameters reproduce the superlattice bands with a very good agreement for the two top bands below the Fermi level and with good agreement for the upper two kagome bands (see Figure and Table ). Plotting the TB parameters as function of the moiré cell's lattice constant shows that all of them are smooth functions (Figure and Table ) and, hence, can easily be parameterized. Details on the TB parameterization are given in the Methods Section and the Supplementary Material.