Recognized for its nutritional and therapeutic use, extra-virgin Argan Oil (EVAO) is frequently adulterated. Selected-Ion Flow-Tube Mass Spectrometry (SIFT-MS) spectra were applied to quantify adulterants (i.e., Argan oil of lower quality (LQAO), olive oil (OO), and sunflower oil (SO)) in EVAO. Four data sets, i.e., using H3O+, NO+, O2+radical dot reagent ions, and the combined data were considered. Soft independent modelling of class analogy (SIMCA), and partial least squares discriminant analysis (PLS-DA) were assessed to distinguish adulterated- from pure EVAO. The effectiveness of SIFT-MS associated with PLS and support vector machine (SVM) regression to quantify trace adulterants in EVAO was evaluated. Variable Importance in Projection (VIP), and interval-PLS (iPLS) were also investigated to extract useful features. Different models were built to predict the EVAO authenticity and the degree of adulteration. High accuracy was achieved. SIFT-MS spectra handled with the appropriate chemometric tools were found suitable for the quality evaluation of EVAO.