Grape variety [Cabernet Sauvignon (CS) and Merlot (M)] effect on the proanthocyanidin composition and sensory perception of wine grapes from Bordeaux vineyards for two successive vintages (2006 and 2007) is reported. The flavan-3-ol monomers [(+)-catechin = C, (-)-epicatechin = EC, (-)-epicatechin-O-gallatte = ECG] and the proanthocyanidin oligomers [dimers B1, B2, B3, and B4 and trimer Cat-Cat-Epi (T)] in grape seed and skin tannin extracts were identified and quantified at harvest. Proanthocyanidin subunit compositions, percentage of galloylation (%G), and percentage of prodelphinidins (%P) as well as mean degree of polymerization (mDP) of the proanthocyanidin fraction were determined. Sensory analysis concerning the astringency and bitterness intensity of the proanthocyanidins of skin and seed tannin extracts was also performed. The results showed that proanthocyanidin composition can be greatly affected by grape variety. For both vintages between CS and M, significant differences were found on mDP (p < 0.05) in seed tannin extracts, whereas in skin tannin extracts, significant differences were observed for %G and %P (p < 0.05). Sensory analysis showed that grape variety influenced neither astringency nor bitterness intensity perception for both skin and seed tannin extracts for the two successive vintages studied. A positive correlation was found between astringency intensity, mDP, and B3 content in skin tannin extracts.