This study compared the use of three sensory and analytical techniques: Quantitative Descriptive Analysis (QDA), Napping, and Gas Chromatography-Mass Spectrometry (GC-MS) for the assessment of flavour in nine unmatured whisky spirits produced using different yeasts. Hierarchical Multiple Factor Analysis (HMFA) showed a similar pattern of sample discrimination (RV scores: 0.895–0.927) across the techniques: spirits were mostly separated by their Alcohol by Volume (ABV). Low ABV spirits tended to have heavier flavour characteristics (feinty, cereal, sour, oily, sulphury) than high ABV spirits, which were lighter in character (fruity, sweet, floral, solventy, soapy). QDA differentiated best between low ABV spirits and GC-MS between high ABV spirits, with Napping having the lowest resolution. QDA was time-consuming but provided quantitative flavour profiles of each spirit that could be readily compared. Napping, although quicker, gave an overview of the flavour differences of the spirits, while GC-MS provided semi-quantitative ratios of 96 flavour compounds for differentiating between spirits. Ester, arenes and certain alcohols were found in higher concentrations in high ABV spirits and other alcohols and aldehydes in low ABV spirits. The most comprehensive insights on spirit flavour differences produced by different yeast strains are obtained through the application of a combination of approaches.