As the world's smallest navigation-grade gyroscope, the nuclear magnetic resonance (NMR) gyroscope has been received widespread attention at home and abroad. The NMR gyroscope determines the angular velocity of the carrier by detecting the change of the spin precession frequency of the nucleus in the magnetic field, and its accuracy is closely related to the uniformity and stability of the magnetic field. The navigation-grade NMR gyroscopes require an fT-level magnetic field environment, while high-efficiency magnetic shielding can generally achieve only 5 to 6 orders of magnitude of magnetic suppression, thus active magnetic compensation is also required. Based on the theoretical analysis of the magnetic field distribution of NMR gyroscope, the lateral magnetic compensation system is analyzed and studied by the mathematical calculation and computer simulation, and the lateral compensation coil is optimized and designed. The magnetic field uniformity of the designed gyroscope lateral compensation system is nearly about 13 times higher than before optimization, meeting the usage requirements of NMR gyroscope. This work provides a theoretical basis and reference value for the design and manufacture of nuclear magnetic resonance gyroscope.