This study presents a pioneering comparison of target stable isotope ratios analysis and sesquiterpene (SH) fingerprinting for authenticating virgin olive oil (VOO) geographical origin. Both methods were selected for being among the most promising targeted and untargeted approaches, respectively. These methods were applied to the same sample set of nearly 400 VOO samples, covering diverse harvest years, cultivars and producers. PLS-DA classification models were developed to differentiate between Italian and non-Italian VOOs, as well as VOOs from three closely located Italian regions. Isotopic models based on bulk δ