The invention provides a cross radiation calibration method and system for a large observation angle sensor. The method comprises steps that a to-be-calibrated image and a reference image are registered, random sampling of each set of corresponding wave bands of the to-be-calibrated image and the reference image is respectively carried out to acquire corresponding calibration points; for each wave band, cross calibration for each pair of calibration points is carried out respectively, a BRDF adjusting coefficient is established as a ratio of a surface bidirectional reflection distribution function of the to-be-calibrated image and a surface bidirectional reflection distribution function of the reference image, and processing is carried out in an iteration mode; for each wave band, points with average mean values greater than a preset threshold are deleted from the cross calibration result, averaging is carried out, and a final radiation calibration coefficient is acquired. The method is advantaged in that BRDF values of the to-be-calibrated image and the reference image can be respectively calculated without a complex model, calculation is simple and stable, strong operationality is realized, and an error caused by introducing auxiliary data for BRDF calculation and influence of abnormal calibration points on the result can be further avoided.