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Composite glasses possessing an amorphous nature and high dielectric constants exhibit properties suitable for optoelectronic and electrochemical applications. Multi-component silica–calcium phosphate glasses doped with 0.5 and 1 mol% of trivalent praseodymium (Pr³⁺) were synthesized using the sol-gel method. The Pr³⁺-doped and undoped glasses were compared at room temperature (300 K) to analyze their electrical variations. Dielectric studies predicted an increase in the dielectric constant and conductivity in the doped samples when compared to the undoped glass. A high dielectric constant of 89.2 was observed in the optimally doped glass at 1 kHz. The value of the capacitance increases to the order of nanofarads as the concentration of Pr³⁺ increases, indicating enhanced storage in the material. The AC conductivity of the highly doped sample evidenced a high value of 2.9 × 10⁻⁵ S/cm at 10 MHz. The Cole–Cole plot of the glasses demonstrated a single flattened semicircle due to the lack of grains. The equivalent circuitry constitutes a constant-phase element (CPE) in series with the parallel circuit of a resistor and CPE. This behavior is indicative of the suitability of the glasses as cathodes. The increase in capacitance with doping in the low-frequency region suggests the use of the glasses as dielectric energy-storage materials in condensers.