The process of recharging heterogeneous lanthanides in SrF2 and BaF2 crystals is studied by parallel measurements of optical absorption spectra and thermodepolarization curves. Electron transfer between lanthanides Yb2+–Nd3+, Eu2+–Yb3+ in SrF2, and between Yb2+–Nd3+, Eu2+–Yb3+, and Yb2+–Dy3+ in BaF2 is studied. Electron phototransfer between lanthanides, registered by a change in the absorption bands of divalent lanthanides, is accompanied by a backward migration of charge‐compensating interstitial fluorine, which is detected by a change in the corresponding thermodepolarization peaks of .