The invention relates to a precise control method of an atom spin SERF (Self-Exchange Relaxation-Free) state for stabilizing an atom spin device, which comprises the following steps that firstly, a precise equation is established for the atom spin SERF state, and a modulation method is adopted to measure the atom spin polarizability to establish a control target; then a control system model as precise as possible is established on the basis of an SERF model, and a parameter identification method is adopted to estimate unknown parameters of the model; and finally, according to the control target, a special structure design control law of the established model is fully used, i.e. the switching time, frequency, orientation and power of laser and the switching time of a modulation magnetic field are optimized, and the atom spin SERF state is precisely controlled in real time in accordance with a quantum control algorithm. By using the precise control method, the atom spin relaxation time is increased, and the problem of instability of scale factors of atom devices such as an atom spin gyroscope and an atom magnetometer based on the atom spin SERF effect is solved. The precise control method can be used for improving the long-time drift precision and the low-frequency sensitivity based on the SERF atom spin device.