The concentration of proanthocyanidins from twenty red wines from cv. Cabernet Sauvignon, five rosé wines from cv. Cabernet Sauvignon and five white wines from cv. Sauvignon Blanc was quantified using four analytical methodologies, and their relationship with the perceived astringency was investigated. Proanthocyanidin concentrations were determined by a methylcellulose precipitation assay, a protein precipitation assay and two colourimetric methods (Bate-Smith and vanillin assay). The four methodologies showed high repeatability but differed widely in proanthocyanidin concentrations. The methylcellulose and protein precipitation assays could not quantify proanthocyanidins in rosé and white wines. The protein precipitation assay gave the lowest concentration of proanthocyanidins in all of the red wines. The methylcellulose precipitation assay (r = 0.7725; r2 = 0.59) and the protein precipitation assay (r = 0.6828; r2 = 0.47) showed a strong correlation with the perceived astringency compared with the colourimetric methods. The strong correlation of the methylcellulose precipitation method with the perceived astringency could be a useful tool to estimate red wine astringency.