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Food frauds present a major problem in the foodstuff industry. Arrowroot and cassava may be targeted in adulteration and falsification processes. Raman analysis combined with chemometric techniques was proposed to identify the mixing and adulteration of these foodstuffs in commercial products. 67 cassava and 5 arrowroot samples were prepared in laboratory. 21 cassava and 5 arrowroot commercial samples were purchased in local stores. Raman assays were performed in the range of 400 to 2300 cm−1. Principal component analysis with K-means clustering was used to identify the adulteration of these products. It was possible to observe the separation of three different groups in the data, these groups labelled group 1, 2 and 3 were correspondent to cassava-like samples, mixed samples, and arrowroot-like samples, respectively. Despite the visual analysis related to sensory characteristics and the visual analysis of each Raman spectrum of cassava and arrowroot not being able to differentiate these foodstuffs, the chemometric approaches with the Raman specters data were able to identify which samples were pure arrowroot, pure cassava and which were mixed products. The proposed approach showed to be an effective tool in the investigation of fraud for arrowroot and cassava.