Calcium uranyl phosphate (CaUP) films were prepared and characterized both chemically and structurally. The electrical behavior of the films, as a solid phase (dry film) and in contact with aqueous solutions of electrolytes containing the generating ions (wet film), was studied by impedance spectroscopy. These last measurements made it possible to determine the contribution of both the bulk film and film/electrolyte interface. For both dry and wet films, the equivalent circuits are a parallel combination of resistance and a nonideal capacitor. Temperature dependence of the impedance of the CaUP solid films was considered, while concentration dependence of the film resistance when it is in contact with the electrolyte solutions was determined. In this case, the contribution of both the bulk film and electrolyte/film interface to the total impedance was also studied.