Spectroscopic data on crystals of rare-earth compounds having structural instability due to the cooperative Jahn–Teller effect are reviewed. Based on an analysis of these data, it is inferred that the dynamic coupling of low-frequency electronic excitations of the rare-earth ions with crystal lattice vibrations plays an essential role in the formation of the low-energy spectra of layered crystals. The role of this coupling in the formation of anomalies of various physical properties of crystals of rare-earth compounds with highly anisotropic structure is examined.