A low-voltage TiO2 capacitor-varistor ceramics doped with Ta2O5 and Nd2O3 was systematically researched. The effect of Nd2O3 on the microstructure, nonlinear electrical properties, and dielectric properties of TiO2-based ceramics was investigated. It was found that an optimal doping composition of 99.20 mol% TiO2-0.10 mol%Ta2O5-0.7 mol% Nd2O3 was obtained with low breakdown voltage of 8.5 v/mm, high nonlinear constant of 4.0, ultrahigh electrical permittivity of 1.07× 105 and low tanδ of 0.39. In view of these electrical characteristics, the ceramics of 99.20 mol% TiO2-0.10 mol%Ta2O5-0.7 mol% Nd2O3 is a viable candidate for capacitor-varistor functional devices. The theory of defects in the crystal lattice was introduced to explain the nonlinear electrical behavior of the Nd2O3-doped TiO2-based varistor ceramics.