The Cross-Track Infrared Sounder (CrIS) on the Suomi National Polar-Orbiting Partnership Satellite is a Fourier transform spectrometer and provides a total of 1305 channels for sounding the atmosphere. Quantifying the CrIS spectral accuracy, which is directly related to radiometric accuracy, is crucial for improving its data assimilation in numerical weather prediction. In this study, a cross-correlation method is used for detecting the effect of Earth-rotation Doppler shift (ERDS) on CrIS observations. Based on a theoretical calculation, the ERDS can be as large as about 1.3 parts in 10(6) (ppm) near Earth's equator and at the satellite scan edge for a field of regard (FOR) of 1 or 30. The CrIS observations exhibit a relative Doppler shift as large as 2.6 ppm for a FOR pair of 1 and 30 near the equator. The variation of the ERDS with latitude and scan position detected from CrIS observations is similar to that derived theoretically, which indicates that the spectral stability of the CrIS instrument is very high. To accurately calibrate CrIS spectral accuracy, the ERDS effect should be removed. Since the ERDS is easily predictable, the Doppler shift is correctable in the CrIS spectra.