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Introduction: Distinguishing and categorizing the origin of garlic are highly significant, considering its widespread use as a flavoring agent. With billions of dollars annually in global trade, garlic is frequently susceptible to fraudulent practices. Methodology: Paper spray ionization mass spectrometry (PS‐MS) was employed to quickly analyze garlic samples from distinct geographic origins: China and Brazil. The so‐generated PS‐MS data were treated with metabolomic multivariate approaches, and the garlic samples from these different geographic regions were easily discriminated. Results: Brazilian garlic was characterized to contain higher levels of amino acids, such as arginine, proline, and valine, and organosulfur compounds, such as allicin, alliin, and l‐γ‐glutamil‐S‐allyl‐l‐cysteine, compared to Chinese garlic. The PS‐MS data were treated employing multivariate approaches, typically used in the metabolomics field, and this protocol was promptly able to discern among both types of samples. Conclusion: Hence, this combined strategy holds promise not only as an effective tool for the authentication of the geographical origin of garlic but also as a powerful means for biomarker discovery. [ABSTRACT FROM AUTHOR]