The flavour of new make spirit (NMS) plays an important role in whisky, which is the final stage before maturation. However, less research has been done on NMS aromas. The aim of this study was to identify aroma compounds that contribute to the sensory properties of NMS and to provide theoretical support for the aroma of NMS prior to maturation. The aromas of three NMS were characterized and evaluated through sensory evaluation experiments. All the samples were produced from different provinces in China. The results of the sensory evaluation showed that sample A (Hunan) had a strong oily aroma, sample B (Sichuan) had a more pronounced sweet aroma, and sample C (Shandong) had a distinctive sulfury flavor and a strong grainy aroma. Headspace solid-phase microextraction combined with comprehensive two-dimensional gas chromatography-time-of-flight mass spectrometry (GC × GC-TOF MS) was used to detect the volatile compounds in the three NMS. The study established a vocabulary to describe the aroma attributes of NMS, which can be categorized into floral (rose, violets, ylang-ylang, jasmine); sweet (honey, burnt sweet); grainy (bake, malt); fruity (banana, citrus, apple, pineapple); oily (fat, nutty); grassy; feinty; sulfury categories. This study will provide a theoretical basis for future research on the aroma of NMS and the control of NMS flavor.