The High-Spectral Infrared Atmospheric Sounder (HIRAS) is a Fourier transform spectrometer onboard the fourth polar-orbiting FengYun 3D satellite (FY-3D). The FY-3D HIRAS provides interferogram measurements of Earth view radiance spectra in three infrared spectral bands at 29 cross-track positions, each with a 2 × 2 array of field of views (FOVs). The HIRAS level 1 radiance data cover the spectral bands from 650 to 1135 cm^-1 [long-wave (LW) band], 1210 to 1750 cm^-1 [mid-wave (MW) band], and 2155 to 2550 cm^-1 [short-wave (SW) band] with a spectral resolution of 0.625 cm^-1. The radiometric calibration algorithm and the methods of refining the nonlinearity (NL) and the polarization correction coefficients on orbit are summarized in this article. The NL correction coefficients are derived by minimizing the spread of the responsivity functions derived from the measurements of the internal calibration target with varying temperatures. The polarization correction coefficients are derived from the cold space observations and the routine Earth scene measurements. The radiometric accuracy is assessed by comparing the HIRAS measurements to the collocated Cross-track Infrared Sounder (CrIS) observations and radiance simulations. The results show that, compared to CrIS, the radiometric differences are about 0.3 and 0.7 K for the LW and MW bands, respectively, and 0.5 K for the CO absorption and window regions in the SW band. The consistency of the radiometric calibration among the four FOVs is estimated to be within 0.2 K for most of the spectral domain. Some remaining issues for the FY-3D HIRAS are also discussed.