A bilayer concept was proposed to adjust the electrical properties of NTC thermistors. The conventional NTC material Ni0.75Mn2.25O4 was chosen as the sensitive layer, and high conductive LaMnO3–Ni0.75Mn2.25O4 composite was chosen as the support layer. The bilayer NTC thermistors were successfully fabricated by classical uniaxial pressing method. After cosintering at 1235°C for 4 h, the two layers adhered well to each other without any cracking or delamination. The resistance decreased linearly with the decrease in the thickness of Ni0.75Mn2.25O4 layer, and the B values varied between 3868 and 3901 K. After annealing at 150°C in air for 500 h, the resistance shifts at 25°C were less than 1%, which mean that the bilayer NTC thermistors had high stability.