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Li–Nb–O amorphous films were deposited onto Si substrates by the radio-frequency magnetron sputtering method in an Ar environment and an Ar(60%)+O₂(40%) gas mixture. A positive effective fixed oxide charge Q_eff having negative, -Q_eff, and positive, +Q_eff, components, exists in the as-grown heterostructures. -Q_eff is located near the substrate/film interface, whereas + Q_eff is determined by a deficit of Li and O (vacancies) in the bulk of Li–Nb–O films. As-grown films crystallized under thermal annealing (TA) at temperatures up to 600 °C and revealed the formation of polycrystalline LiNbO₃. TA at about 520 °C resulted in the formation of the second phase LiNb₃O₈, increasing + Q_eff, and compensating -Q_eff entirely. The dielectric constants of the as-grown films exhibit two peaks at the annealing temperatures of 450 °C and 550 °C, which are attributed to the total crystallization and recrystallization of the LN films under TA, respectively. © 2020 The Authors