The relationship between the crystal structure of Bi2O3 and the recovery of the electrical degradation of ZnO varistors was investigated. The evaluation methods used were analysis of the voltage-current (V-I) characteristics, scanning electron microscopy (SEM), energy-dispersion X-ray spectroscopy (EDX), and X-ray diffraction (XRD) measurements. The electrical degradation was estimated by the nonlinearity of the V-I characteristics. A marked recovery of the nonlinearity of the V-I characteristics was observed for a sample having the crystal structure of δ-type Bi2O3. It is speculated that the electrical degradation is markedly recovered for optimum conditions of both the amount and the crystal structure of the added Bi2O3, because, for samples sintered for a long time, the recovery speed is shorter than that for samples sintered for a shorter time. During long-time sintering, the amount of Bi2O3 decreased because of evaporation. No change of the crystal structure of Bi2O3 was observed upon repeated the electrical degradation and the recovery. It is suggested that another mechanism apart from the diffusion of oxygen ions through the grain boundaries of ZnO particles contributes to the electrical degradation and recovery of the nonlinearity of V-I characteristics.