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The influence of the CuO–TiO2 phase (CT) on dielectric properties of the CCTO ceramic was investigated. CaCuXTiYO12 (CCXTYO) powders were prepared based on the coprecipitated method, where 2.70 ≤ x ≤ 3.30 and 3.25 ≤ y ≤ 4.75. XRD patterns confirmed the presence of CCTO and also the secondary phases as CuO, TiO2, and CaTiO3 for each sample and aided in its quantification. Scanning Electron Microscopy (SEM) shows secondary phases evolution in the grain boundaries, and its influence on size and morphology of the grains. Impedance spectroscopy measurements showed that the ceramics with lower amount of CuO and TiO2 phases (CT/deficient ceramics) exhibited the highest ε′ values (2.1 × 104 at 1 kHz for CC2.9T3.75O ceramic). Also, CT/deficient ceramics showed lower tanδ values (0.090 at 1 kHz for CC2.9T3.75O ceramic) than ceramics prepared with excessive CuO–TiO2 phase (0.241 at 1 kHz for CC3.1T4.25O ceramics). The deficiency of CuO and TiO2 phases associated with high percentage of CCTO and CaTiO3 phases resulted in ceramics with the higher ε′ values. [ABSTRACT FROM AUTHOR]