Inelastic neutron scattering (INS) was used to study dynamics of the hydrogen atoms in natural 2M1 muscovite in the 150–1200 cm−1 energy range. The resultant INS spectra are interpreted by means of solid-state density functional theory calculations covering both normal mode analysis and molecular dynamics. While signatures of the Al-O-H bending modes were found over the whole energy transfer range, the dominant contributions were observed between 800–1000 cm−1. The modes assigned to the in-plane movements of the respective hydrogen atoms are well defined and always appear at high energies. In contrast, the modes corresponding to the out-of-plane movements are spread over large energy transfer ranges, extending down to the region of external (lattice) modes. The positions of the high-energy modes contributing to the INS band at ~907 cm−1 depend on the distance of respective hydrogen atoms to the nearest oxygen atom of the basal net and its polarity.