TbFeO3 ceramics were prepared via conventional solid-state reaction route. By means of the complex dielectric permittivity, electric modulus, and impedance analysis, the high-temperature dielectric properties of TbFeO3 were investigated in the temperature range from 300 to 1073K and frequency range of 102–107Hz. Rich dielectric phenomena, including three dielectric responses (R1–R3), a relaxor-like dielectric anomaly and negative capacitance were found in the order of ascending temperature. The low-temperature relaxation (R1) near room temperature is caused by the surface-layer effect. The high-temperature relaxations R2 and R3 were argued to be related to the dipolar and Maxwell–Wagner relaxation, The anomaly is confirmed to be caused by the negative capacitance effect.