AbstractPaleomagnetic analyses have suggested that the lunar magnetic field underwent a significant change from 4.25 to 3.19 Ga, indicating the rapid transition of the lunar dynamo mechanism. We used the van der Pauw (vdP) method to measure the electrical resistivity of Fe‐S‐P alloys under conditions relevant to the lunar core and estimated the thermal conductivity of the Fe‐S‐P lunar core. These values were incorporated into thermal and dynamo models to investigate the evolution of the lunar core. Our model indicates that the inner core began to grow as early as 4.35 Ga, the solidification regime switched at 3.50 Ga, and the thermal dynamo ceased between 3.78 and 3.51 Ga. The cessation of the dynamo could be due to a low buoyancy flux and insufficient entropy dissipation. Thermal and compositional dynamos cannot sustain the ancient strength of the Moon's magnetic field, and require other energy sources.