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This study presents the dielectric properties of a barium titanate–gadolinium ferrite composite material, obtained through a solid-state reaction method. The aim of this research was to create a composite material with enhanced dielectric properties compared to each individual component, and to investigate the electrical properties of the composites, using impedance spectroscopy. The structural and morphologic properties were analyzed using X-ray diffraction and scanning electron microscopy, respectively. Impedance spectroscopy measurements were performed over a wide frequency range (100–0.1 GHz) and temperature (45–170 °C) to evaluate the electrical behavior of the material. The dielectric relaxations were analyzed using the Havriliak–Negami function, and the key electrical parameters such as relaxation frequency, dielectric strength, and electrical conductivity were extracted. Several relaxation processes were identified, which depend on the mixture of the initial titanate and ferrite materials, and a correlation between structural, morphologic, and electrical properties was exposed. The sample with the highest dielectric constant was the 25 wt% gadolinium ferrite composite, with ε′ close to 240 and loss tangent values below 0.1, affording it the more appropriate composition for energy storage devices such as lead-free dielectric capacitors. [ABSTRACT FROM AUTHOR]