The on-orbit radiometric calibration of spaceborne sensors is the foundation of quantitative remote sensing, and the calibration accuracy directly affects the quality of quantitative remote sensing products. The wide swath of the Chinese Ocean Color and Temperature Scanner (COCTS) onboard the HY-1C satellite makes it difficult to ignore errors caused by viewing angles during calibration. Thus, this article proposes a cross-calibration method based on the bottom-of-atmosphere (BOA) and top-of-atmosphere (TOA) spectral band adjustment factors (SBAFs). This method cross calibrates the COCTS sensor after correcting viewing geometry and radiometric differences. It is based on the Sentinel-3/ocean and land color instrument (OLCI) sensor. First, time-series data from the OLCI sensor were used to select calibration points in the Dunhuang area. Subsequently, the bidirectional reflectance distribution function (BRDF) for each corresponding spectral band of the OLCI sensor was constructed point by point. Next, the BOA and TOA SBAFs were calculated using the interpolated continuous spectra obtained from MOD09GA products. After correcting for the BRDF and SBAF, cross calibration between COCTS and OLCI was achieved. The results showed that the BOA SBAF model achieved higher precision calibration coefficients than the TOA SBAF model, with errors in each band below 5.76%. The proposed method can provide technical support for the cross calibration of wide-swath sensors.