In order to detect contaminants on surface, a method for surface contamination detection was developed based on multi-angle infrared differential absorption spectra. As contaminants′ absorption ability varied with measurement angles, the spectral features of contaminants could be extracted from multi-angle observations. Firstly, multi-angle measurement model of chemical contaminants was introduced. Then three typical compounds: poly (dimethylsiloxane), triethyl phosphate and methyl salicylate were measured both in laboratory and field on different substrates. The results showed that, with multi-angle infrared differential absorption spectra, this method could extract directly spectral features of contaminants both in laboratory and field on typical surfaces, and spectral features of contaminants got more distinct with more smooth substrate and larger difference between two incidence angles employed. This method had application potential in immediate responding for chemical contaminants detection.