The engineering of grain boundary barriers plays a critical role in the performance of ZnO-based varistor ceramics. The formation and height of these barriers are influenced by sintering conditions, cooling processes, and dopant selection. While Bi2O3 is known to induce grain boundary effects in ZnO varistor ceramics, the presence of unsaturated transition metal oxides is essential for enhancing the grain boundary barrier. Unfortunately, this process requires the collaboration of multiple unsaturated transition metal oxides, which results in the complexity involved in formulating ZnO varistors and hinders their further development. In this work, a novel high nonlinear coefficients low-voltage ZnO-based varistor ceramics was prepared through Aluminum Nitride (AlN) doped. This successful design enhances the nonlinear conductivity properties in ZnO varistor ceramics, resulting in superior varistor performance. Specifically, the AlN-doped ZnO varistor ceramics (x = 1 mol%) exhibit an excellent nonlinear coefficient of 49.58, comparable to that of other multicomponent-doped ZnO-based varistor ceramics. This research offers a new practical strategy for developing high-performance low-voltage ZnO-based varistor ceramics.