Wheat has played an important role in human agriculture since ancient times. Increasing rates of processed wheat product fabrication require more and more laboratory studies of product quality. This, in turn, requires the use, in production and in field conditions, of sufficiently accurate, fast and relatively low-cost quality control methods, including the detection of fungal diseases. One of the most widespread fungal diseases of wheat in the world is ergot caused by the fungi genus Claviceps. Optical methods are promising for this disease identification due to the relative ease of implementation and the possibility of performing fast analyses in large volumes. However, for application in practice, it is necessary to identify and substantiate characteristic spectral markers that make it possible to judge the sample contamination. In this regard, within the framework of this study, the methods of IR absorption spectroscopy in the MIR region and reflection spectroscopy in the UV-vis-NIR ranges, as well as luminescence spectroscopy, were used to study ergot-infected grains of winter wheat of the “Moskovskaya 56” cultivar. To justify the choice of the most specific spectral ranges, the methods of chemometric analysis with supervised classification, namely PCA-LDA and PCA-SVM, were applied. The possibility of separating infected grains according to the IR absorption, reflection spectra in the UV-vis-NIR ranges and visible luminescence spectra was tested.