The origin of giant dielectric relaxation behavior and related electrical properties of grains and grain boundaries (GBs) of W6+-doped CaCu3Ti4O12 ceramics were studied using admittance and impedance spectroscopy analyses based on the brick–work layer model. Substitution of 1.0 at. % W6+ caused a slight decrease in GB capacitance, leading to a small decrease in the low-frequency dielectric constant. Surprisingly, W6+ doping ions have remarkable effects on the macroscopic dielectric relaxation and electrical properties of grains. X-ray photoelectron spectroscopy analysis suggested that the large enhancements of grain resistance and conduction activation energy of grains for the W6+-doped CaCu3Ti4O12 ceramic are caused by reductions in concentrations of Cu3+ and Ti3+ ions. Considering variation of dielectric properties together with changes in electrical properties of the W6+-doped CaCu3Ti4O12 ceramic, correlation between giant dielectric properties and electrical responses of grains and GBs can be described well by the internal barrier layer capacitor model. This model can ascribe mechanisms related to giant dielectric response and relaxation behavior in CaCu3Ti4O12 ceramics.

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A novel concept to simultaneously modify the electric responses of the grain and grain boundaries of CaCu3Ti4O12 ceramics was proposed, involving doping with F− anions to improve the giant dielectric properties.

The dielectric and non‐Ohmic properties of Na1/2Y1/2Cu3Ti4O12 ceramics sintered under various conditions to obtain different microstructures were investigated. Microstructure analysis confirmed the presence of Na, Y, Cu, Ti, and O and these elements were well dispersed in the microstructure. Na1/2Y1/2Cu3Ti4O12 ceramics exhibited non‐Ohmic characteristics with large nonlinear coefficients of about 5.7–6.6 irrespectively of sintering conditions. The breakdown electric field of fine‐grained ceramic with the mean grain size of ≈1.7 μm (≈5600 V/cm) was much larger than those of the course‐grained ceramics with grain sizes of ≈9.5–10.4 μm (≈1850–2180 V/cm). Through optimization of sintering conditions, a low loss tangent of about 0.03 and very high dielectric permittivities of 18 000–23 000 with good temperature stability were successfully accomplished. The electrical responses of the grains and grain boundaries can, respectively, be well described using admittance and impedance spectroscopy analyses based on the brickwork layer model. A possible mechanism for the origin of semiconducting grains is discussed. The colossal dielectric response was reasonably described as closely correlated with the electrically heterogeneous microstructure by means of strong interfacial polarization at the insulating grain‐boundary layers. The non‐Ohmic properties of Na1/2Y1/2Cu3Ti4O12 ceramics were primarily related to their microstructure, i.e., grain size and volume fraction of grain boundaries.

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