This study was conducted during the 2014 and 2015 vintages on Vitis vinifera L. cv. Merlot and Cabernet Gernischt to investigate whether natural variation in berry size could affect grape aromatic compounds. Grape berries were separated into three size categories based on their diameter: small, middle and large. The results showed that berry size exerted a significant influence on the volatile profiles of both winegrape varieties. Hierarchical clustering analysis demonstrated that the volatile profiles of middle berries were different from those of large and small berries. Middle berries had the greatest abundance of aroma compounds, followed by small and large berries. Especially, C6/C9 compounds, norisoprenoids, terpenoids showed markedly different concentrations among differently sized Merlot berries and C6/C9 compounds, terpenoids among differently sized Cabernet Gernischt berries. Middle berries of both grape varieties may possess the greatest intensity of fresh-green, fruity and floral aromas due to the high odour activity values (OAVs) of decanal, hexanal, (E)-2-hexenal, (E)-β-damascenone and β-ionone in middle sizes of Merlot berries and the high OAVs of (E)-2-hexenal and (E)-β-damascenone in middle sizes of Cabernet Gernischt berries. This knowledge could be important for winemakers to conduct targeted berry sorting, thereby improving the aromatic quality of grapes.