The authenticity of products labeled as virgin olive oil is of great importance from commercial and health aspects. The combination of Fourier transform-Raman (FT-Raman) spectroscopy with multivariate procedures has been used for predicting the level of adulteration in a set of virgin olive oil samples that were adulterated with soybean, corn, and raw olive residue (olive pomace) oils at 1, 5, and 10%, respectively. Six genuine virgin olive oil samples, differing in their chemical composition, were selected from a set of 1428 European samples. The best result in prediction of adulteration was an adjusted R(2) value of 0.964, determined by regression on principal components (PCR), giving 100% correct discrimination between genuine and adulterated samples and 91.3% correct classifications at different adulteration levels.