In order to meet the demand of large turning angle range in optoelectronic countermeasure equipment, the calibration technology of two-dimensional large-angle fast steering mirror angle measurement system based on eddy current sensors is investigated, and the two-dimensional large-angle fast steering mirror calibration system is designed. The angular measurement principle of the calibration system is analyzed, and model construction and experimental testing are carried out by combining the two methods through theoretical and residual analyses of polynomial fitting and bilinear interpolation calibration models. The results show that the overall error of applying the bilinear interpolation fitting method is less than 30 ″in the angular range of ±7 °(±25200 ″). Comparison experiments with the traditional polynomial fitting and bilinear interpolation show that the bilinear interpolation fitting method has a smaller calibration error, higher localization accuracy, and is more suitable for two-dimensional large-angle fast reflector calibration.