The FFT images given in Fig. are especially worth noting. We see that in addition to the two sets of 100 Bragg spots defining a twist angle, there exist several extra spots, which are located symmetrically with respect to the center spot in the inner region of the 100 spots. These extra spots have not been explicitly reported in previous HRTEM observations on MSLs. We also found that these inner spots are not observed in the TEM image of the twisted hBN layers with hydrocarbon adsorbates (Fig. ). This allows us to confirm that clean and strain-free samples are necessary for the observation of the inner spots. Since these inner spots have larger d-spacings than the 100 spots, the presence of these spots could be correlated to the existence of longer periodicity or longer interatomic correlations pertinent to the respective moiré structures. This consideration is supported by the inspection of the positions of the extra spots ke in reciprocal space. It has been revealed that ke can be found by connecting the two Bragg spots belonging to the different layers and translating the obtained vectors to the center of the diffraction pattern, as demonstrated in Fig. . The relationship can be written as, where ke = G1 G2, where Gi (i = 1, 2) represents the reciprocal vectors from two different layers. Thus, these extra spots most likely result from some electron scattering processes related to the interlayer correlations. Here, one should remind that the contrast in HRTEM images is proportional to the projected specimen potential, convoluted with the impulse response of the instrument. Note, however, that diffraction peaks due to moiré structures cannot be observed when acquired at typical TEM electron energies (60300 keV), provided that the projected specimen potential consists only of the potentials of individual atoms in the respective layers (see 'Intensity of moiré peaks in diffraction pattern' section in the Supporting Information). We hence assume that the observed extra diffraction spots are not originated from the atomic potentials within the layers, but from a well-characterized moiré potential created in the interlayer region.