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Herein, the structural and electrical properties of TbFeO3 ceramic, prepared by the conventional mixed‐oxide reaction method are investigated. The compound crystallizes in an orthorhombic crystal system. The multiple valence states of Tb and Fe in the compound are confirmed by X‐ray photoelectron spectroscopy. An exciting broad dielectric peak at around 160 °C with a peak value of 48 800 at 100 Hz is observed, whose origin seems to be intrinsic in nature and is based on the coexistence of multiple valence states of Tb, due to the use of Tb4O7 as the precursor material. A hysteresis loop is recorded at various temperature points from the ferroelectric to paraelectric transition at the temperature corresponding to the peak of the observed dielectric anomaly. The loss tangent is resolved to identify contributions from the Debye‐type relaxation for both grain and grain boundary effects and that of DC conductivity. The conduction mechanism associated with grain and grain boundary is explained using different models.

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