237Np (≃2.14 × 106 yr half-life) is potentially applicable in studies on nuclear safeguards and radioactive waste migration. The atomic ratio of 237Np/U in nature is 10−12 or even lower, depending strongly on the integral neutron flux received by the material. As an ultra-sensitive technique, accelerator mass spectrometry (AMS) is the best for measuring ultratrace 237Np. By extracting negative molecular ions NpO– from the oxide sample using 238UO– and 208Pb16O2– pilot beams for the simulation of 237Np ion transport, identifying the interference isotopes by high-resolution dedicated injector, electrostatic analyzer, and time of flight (TOF) detector, a method for AMS measurement of 237Np was set up on the HI-13 accelerator at the China Institute of Atomic Energy (CIAE). A sensitivity of <10–11 has been achieved for the isotopic ratio 237Np/238U.